Clemens Spinnler, Liang Zhai, Giang N. Nguyen, Julian Ritzmann, Andreas Dirk Wieck, Arne Ludwig, Alisa Javadi, Doris E. Reiter, Paweł Machnikowski, Richard John Warburton, Matthias C. Löbl
In a radiative Auger process, optical decay leaves other carriers in excited states, resulting in weak red-shifted satellite peaks in the emission spectrum. The appearance of radiative Auger in the emission directly leads to the question if the process can be inverted: simultaneous photon absorption and electronic demotion. However, excitation of the radiative Auger transition has not been shown, neither on atoms nor on solid-state quantum emitters. Here, we demonstrate the optical driving of the radiative Auger transition, linking few-body Coulomb interactions and quantum optics. We perform our experiments on a trion in a semiconductor quantum dot, where the radiative Auger and the fundamental transition form a Λ-system. On driving both transitions simultaneously, we observe a reduction of the fluorescence signal by up to 70%. Our results suggest the possibility of turning resonance fluorescence on and off using radiative Auger as well as THz spectroscopy with optics close to the visible regime.
In a radiative Auger process, optical decay leaves other carriers in excited states, resulting in weak red-shifted satellite peaks in the emission spectrum. The appearance of radiative Auger in the emission directly leads to the question if the process can be inverted: simultaneous photon absorption and electronic demotion. However, excitation of the radiative Auger transition has not been shown, neither on atoms nor on solid-state quantum emitters. Here, we demonstrate the optical driving of the radiative Auger transition, linking few-body Coulomb interactions and quantum optics. We perform our experiments on a trion in a semiconductor quantum dot, where the radiative Auger and the fundamental transition form a Λ-system. On driving both transitions simultaneously, we observe a reduction of the fluorescence signal by up to 70%. Our results suggest the possibility of turning resonance fluorescence on and off using radiative Auger as well as THz spectroscopy with optics close to the visible regime.
Quantum optics provides a fundamental framework for understanding the interaction between light and matter at the quantum level. Recently, it has been shown that under incoherent pumping, the resonance fluorescence spectrum dramatically changes. Engineering the resonance fluorescence spectrum paves the way towards solid-state-based single-photon sources. In this paper, we start by reviewing and reproducing some of the results concerning the resonance fluorescence spectrum, single-photon sources, dressed-state lasers, and luminescence spectrum of a quantum dot in a microcavity. Photon correlations in quantum optical systems and spectral properties of radiation emitted by atomic and semiconductor systems interacting with external fields are investigated. The well known Mollow triplet structure of the emission spectrum is discussed, together with the role of dressed states in explaining the origin of the three spectral peaks. Furthermore, the luminescence spectra of quantum emitters coupled to microcavities are reviewed. The numerical results presented here contribute to the theoretical understanding of resonance fluorescence, photon correlations, and engineered emission in quantum optical systems. These studies highlight the rich physical properties arising from light matter interaction at the quantum level and demonstrate their relevance for emerging quantum technologies.
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.
Single semiconductor quantum dots, which are considered as two-level systems in the artificial atom model, are promising structures for the realization of integrated devices such as single photon sources for quantum information applications. However, contrary to genuine atoms, they are condensed matter systems which suffer from the coupling to their solid environment, leading to a degradation of the coherence of the emitted photons. One possibility to avoid this coupling, thereby improving the coherence of the photons until the one imposed by the radiative limit T2 = 2T1, is to perform strictly resonant excitation of a quantum dot at low temperature. Using an experimental setup that spatially decouples the excitation and detection paths, we showed that a fine control of the electrostatic environment related to the nanostructures residual doping remains a major challenge to answer the widely encountered problem of the inhibition of the resonance fluorescence of a quantum dot. Meanwhile, thanks to quantum optics experiments and high resolution optical spectroscopy, we demonstrated that the resonant Rayleigh scattering regime where quantum dots emit single photons with the laser coherence time, paves the way to the development of "ultra-coherent" sources of single photons with high degrees of indistinguishability. In this regime where the laser tailors the coherence of the photons and where the radiative limit becomes a secondary requirement, two photons emitted successively by the same quantum dot are indistinguishable on time scales never obtained before for a solid nano-emitter (up to ten nanoseconds, comparing to the carriers lifetime and decoherence time of about a hundred of picoseconds).
The coherent interaction between a two-level system and electromagnetic fields serves as a foundation for fundamental quantum physics and modern photonic quantum technology. A profound example is resonance fluorescence, where the non-classical photon emission appears in the form of a Mollow-triplet when a two-level system is continuously driven by a resonant laser. Pushing resonance fluorescence from a static to dynamic regime by using short optical pulses generates on-demand emissions of highly coherent single photons. Further increasing the driving strength in the dynamical regime enables the pursuit of exotic non-classical light emission in photon number superposition, photon number entanglement, and photon bundle states. However, the long-sought-after spectrum beyond the Mollow-triplet, a characteristic of dynamic resonance fluorescence under strong driving strength, has not been observed yet. Here we report the direct observation and systematic investigations of dynamic resonance fluorescence spectra beyond the Mollow-triplet in a solid-state cavity quantum electrodynamic system. The dynamic resonance fluorescence spectra with up to five pairs of side peaks, excitation detuning induced spectral asymmetry, and cavity filtering effect are observed and quantitatively modeled by a full quantum model with phonon scattering included. Time-resolved measurements further reveal that the multiple side peaks originate from interference of the emission associated with different temporal positions of the excitation pulses. Our work facilitates the generation of a variety of exotic quantum states of light with dynamic driving of two-level systems.
Abstract The coherent interaction between a two-level system and electromagnetic fields serves as a foundation for fundamental quantum physics and modern photonic quantum technology. A profound example is resonance fluorescence, where the non-classical photon emission appears in the form of a Mollow-triplet when a two-level system is continuously driven by a resonant laser. Pushing resonance fluorescence from a static to dynamic regime by using short optical pulses generates on-demand emissions of highly coherent single photons. Further increasing the driving strength in the dynamical regime enables the pursuit of exotic non-classical light emission in photon number superposition, photon number entanglement, and photon bundle states. However, the long-sought-after spectrum beyond the Mollow-triplet, a characteristic of dynamic resonance fluorescence under strong driving strength, has not been observed yet. Here we report the direct observation and systematic investigations of dynamic resonance fluorescence spectra beyond the Mollow-triplet in a solid-state cavity quantum electrodynamic system. The dynamic resonance fluorescence spectra with up to five pairs of side peaks, excitation detuning induced spectral asymmetry, and cavity filtering effect are observed and quantitatively modeled by a full quantum model with phonon scattering included. Time-resolved measurements further reveal that the multiple side peaks originate from interference of the emission associated with different temporal positions of the excitation pulses. Our work facilitates the generation of a variety of exotic quantum states of light with dynamic driving of two-level systems.
Intersubband transitions are unbound electronic transitions of doped quantum wells, semiconductors heterostructures with a planar symmetry. I theoretically studied the fluorescence of a strongly pumped intersubband transition, finding that the many electron nature of such a system leads to a modification of the usual Mollow triplet. In particular, the intensity of the central peak in the fluorescence spectrum becomes a function of the electron coherence, allowing access to the coherence time of a quasi two-dimensional electron gas through a fluorescence intensity measurement. Moreover, while transitions between the two states of the ac Stark-split doublet are forbidden in centrosymmetric systems, and thus almost impossible to observe in experiments performed with atoms they become allowed in asymmetric quantum wells, in which the wave function symmetry can be broken. I developed a many-body theory describing also this intradoublet emission, showing that by using doped asymmetry, the emission can be orders of magnitude higher than in previously studied systems. This opens the way to the realization of monolithic and tunable terahertz emitters since the Rabi frequency at which this emission occurs lies in the terahertz range and can be tuned by the pump power. Finally, I have investigated if superfluorescence can occur in intersubband transitions. In order to do so I used a general quantum master equation that includes dephasing and nonradiative emission to model the many-body system in solid state. Performing a second-order approximation allowed to obtain a closed system of equations that were studied analytically and numerically, verifying that in the regimes characteristic of intersubband transitions cooperative effects leading to powerful bursts of light could be observed experimentally.