The fluorescence of a single dipole excited by an intense light pulse can lead to the generation of another light pulse containing a single photon. The influence of the duration and energy of the excitation pulse on the number of photons in the fluorescence pulse is studied. The case of a two-level dipole with strongly damped coherences is considered. The presence of a metastable state leading to shelving is also investigated.
The fluorescence of a single dipole excited by an intense light pulse can lead to the generation of another light pulse containing a single photon. The influence of the duration and energy of the excitation pulse on the number of photons in the fluorescence pulse is studied. The case of a two-level dipole with strongly damped coherences is considered. The presence of a metastable state leading to shelving is also investigated.
Due to their excellent optical properties, quantum dots are promising for applications in photonic quantum technologies. For on-demand single-photon generation, a two-level system given by an excitonic transition is typically excited with a resonant laser pulse of area π. This prepares the two-level system in its excited state from where it spontaneously emits a single photon. However, emission that occurs already during the presence of the laser pulse allows for re-excitation and, thus, multi-photon emission which limits the single-photon purity [1]. In contrast, when exciting the system with a pulse of area 2π, the system is expected to be returned to the ground state. However, in this case emission during the presence of the pulse is most likely to occur when the system is in its excited state – exactly after an area of π has been absorbed. This restarts the Rabi oscillation with a pulse area of π remaining in the pulse which leads to re-excitation with near-unity probability and the emission of a second photon within the excited state lifetime [2,3]. Finally, we present the generation of single photons with ultra-low multi-photon probability [4]. Using two-photon excitation of the bi-exciton suppresses re-excitation and improves the single photon purity by several orders of magnitude for short pulses. [1] K. A. Fischer, et al., New J. Phys. 18, 113053 (2016) [2] K. A. Fischer, et al., Nature Physics 13, 649-654 (2017) [3] K. A. Fischer, et al., Quantum Sci. Technol. 3, 014006 (2017) [4] L. Hanschke et al., arxiv: 1801.01672 (2018)
The generation of non-classical states of light [1] is an important scientific challenge with many potential applications. For example, squeezed states of light [2] have generated much interest in the past decade, because measurements can be performed with noise levels that are lower than those available with classical light. A particularly novel non-classical source of light is a triggered single-photon source: a source that has the property to emit with a high degree of certainty one (and only one) photon at a user-specified time. Such a deterministic source of single photons can be important for quantum information processing [3], quantum cryptography [4] and certain quantum computation problems [5]. A single quantum emitter such as a molecule or an atom is a good potential source because it can emit only one photon at a time. The emitted light is antibunched [6, 7] and consists of single photons separated by random time intervals, which depend on the excited state lifetime and on the pumping rate. Thus triggered emission of single photons can be obtained with controlled excitation of a single emitter. The first demonstration of a single photons source [8] using a single molecule in a solid is based on a rapid adiabatic passage method [9] to excite the molecule. In the effective spin picture, the Bloch vector follows the driving magnetic field adiabatically if the laser-molecule frequency detuning is swept slowly through the resonance. Since the passage inverts the field, the system goes from the ground to the excited state. From this fluorescent state the molecule can emit only a single photon. The molecular resonance is swept by Stark effect at fixed laser frequency. This is done easily by applying a radio frequency electric field to the molecule. The results showed photon states with statistics that differ radically from those of coherent states. But this method requires cryogenic temperatures (2K) since narrow zero phonon lines are needed for the adiabatic following. At room temperature a source of triggered single photons based on the concept of pulsed optical excitation of a single highly fluorescent molecule has been demonstrated [10]. A short pulse of green laser light pumps the molecule from the ground state to a vibronically excited level of the first electronic excited state. After fast (ps) relaxation to the lowest electronic excited state, the molecule subsequently emits a single photon. A frequency-doubled mode-locked Nd-YAG laser is used to pump highly stable single terrylene molecules contained in a p-terphenyl molecular crystal where they are protected from exposure to diffusing quenchers (such as oxygen). The result shows that the photons are emitted after the laser pulses at times separated by the laser repetition time within the lifetime of terrylene in p-terphenyl. Since the pump pulse width is very short compared to the fluorescence lifetime, the probability of two (or more) photon emission per pulse is always zero. At the maximum laser power, 90% of the laser pulses lead to a single photon emission. The parameters of this source (repetition rate and single photon generation probability) were limited only by the laser system used; nevertheless, this performance already surpasses that of previous work. The high performance combined with the vanishing two photon emission probability and the simplicity of this source suggests that it can be considered for a variety of quantum optical experiments and for secure quantum cryptography [11]. Semiconductor quantum dots (QD) are other potential systems for single photon generation [12]. QDs are often referred to as “artificial atoms” because many of their optical properties, such as ultranarrow transitions, arise from discrete, atomic-like energy levels [13, 14]. To reinforce this analogy a study of the photon antibunching in this system was needed. QDs differ from atoms and molecules since the creation of multiple excitons is possible in QDs. Consequently, if two electron-hole pairs can radiatively recombine, the simultaneous emission of two photons from a QD is then possible. Thus different regimes of photon statistics were expected because the probability of multiple exciton creation depends on excitation intensity. The fluorescence intensity correlation function of a single CdSe quantum dot has been investigated [15] using a coincidence setup (start-stop experiment). A strong photon antibunching has been observed over a large range of intensities (0.1-100 kW/cm2). The lack of coincidence at zero time delay indicates a highly efficient Auger ionization process [16], which suppresses multi-photon emission in these colloidal quantum dots. This result shows that room temperature single photon sources can be achieved with colloidal nanoparticles.
Photon emission from a single molecule at room temperature exhibits nonclassical features. Continuous wave fluorescence excitation provides antibunching in the emitted photons sequence as a signature of the property to only emit one photon at a time. A short pulsed excitation can then produce single photons on demand, with an overall quantum efficiency up to 4.5% in our experimental setup. Direct measurement of the Mandel parameter Q ( T ) for an observation period of duration T follows a subpoissonian statistics on short time scale and superpoissonian statistics on longer time scale. The latter is attributed to blinking in the fluorescence due to the occurence of a metastable molecular triplet state.
We consider a single-photon bound–bound and bound–free transitions induced by short, coherent laser pulses. Fluorescence energy spectra are calculated. In the case of the fluorescence to a side level, a number of analytic results are presented. For the resonance-fluorescence case the compact Bloch-like equations are derived for the ionization to an autoionization resonance and numerically analyzed. The multipeak structure of the spectra previously found in the simplified models is shown to be a universal feature. The number of maxima of the spectrum increases with the area of the pulse.
It has been observed experimentally [H.R. Xia, C.Y. Ye, and S.Y. Zhu, Phys. Rev. Lett. 77, 1032 (1996)] that quantum interference between two molecular transitions can lead to a suppression or enhancement of spontaneous emission. This is manifest in the fluorescent intensity as a function of the detuning of the driving field from the two-photon resonance condition. Here we present a theory that explains the observed variation of the number of peaks with the mutual polarization of the molecular transition dipole moments. Using master equation techniques we calculate analytically as well as numerically the steady-state fluorescence, and find that the number of peaks depends on the excitation process. If the molecule is driven to the upper levels by a two-photon process, the fluorescent intensity consists of two peaks regardless of the mutual polarization of the transition dipole moments. If the excitation process is composed of both a two-step, one-photon process and a one-step, two-photon process, then there are two peaks on transitions with parallel dipole moments and three peaks on transitions with antiparallel dipole moments. This latter case is in excellent agreement with the experiment.