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Quantum Electronics and Laser Science Conference

Triggered single photons from a quantum dot

Charles Santori, Matthew A. Pelton, Glenn S. Solomon, Yseulte Dale, Y. Yamamoto

Published Nov 13, 2002• 13 citations
Publisher

Abstract

Summary form only given. A source of single photons, each arriving within a known time interval, would be useful in the new field of quantum cryptography, where security from eavesdropping requires that only one photon be sent at a time. While other recent efforts to generate single photons have relied on saturated absorption in a single quantum emitter such as a molecule our method takes advantage of the emission properties of a single emitter, an InAs dot. When a laser pulse creates multiple electron-hole pairs (excitons), the last pair to recombine creates a photon at a unique wavelength, which can be spectrally separated from the others. This is because Coulomb interactions shift the emission wavelength when multiple excitons are present.

DOI
10.1109/qels.2001.962045

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Summary form only given. A source of single photons, each arriving within a known time interval, would be useful in the new field of quantum cryptography, where security from eavesdropping requires that only one photon be sent at a time. While other recent efforts to generate single photons have relied on saturated absorption in a single quantum emitter such as a molecule our method takes advantage of the emission properties of a single emitter, an InAs dot. When a laser pulse creates multiple electron-hole pairs (excitons), the last pair to recombine creates a photon at a unique wavelength, which can be spectrally separated from the others. This is because Coulomb interactions shift the emission wavelength when multiple excitons are present.
A standard laser produces a coherent state of light with a Poissonian photon number distribution. Generation of single photons on demand is a key requirement for quantum key distribution and quantum information processing systems based on photonic qubits. One of the generation schemes for single photons is to use a single semiconductor quantum dot embedded in a monolithic microcavity. An optical pump pulse or electrical pump pulse generates more than one electron–hole pairs in a quantum dot. Those electron–hole pairs recombine to generate photons one by one via spontaneous emission. The last photon emitted from a quantum dot has a unique wavelength, differing from the other photons, because the multiparticle interaction inside a quantum dot modulates an emission wavelength. One can selectively extract this last photon by a narrow band optical filter, so that single photons are extracted from the system no matter how many electron–hole pairs are injected into the quantum dot initially.
Semiconductor Quantum dots are potentially an attractive source of non-classical light. They can confine bound electron-hole pairs, excitons, in all three spatial dimensions giving them discrete optical emission energies, much like the electronic states in atomic systems. The semiconductor nature of the system allows quantum dots to be integrated into complicated device structures including optical cavities [1] and electrical injection [2]. The radiative exciton emission from a semiconductor quantum dot can provide the simplest form of quantum light, a single photon source [2]. The finite re-excitation time following the radiative decay of an exciton in a quantum dot prevents the dot from emitting more than one photon if excited with a short optical or electronic pulse. In a similar fashion excitation of the biexciton state, consisting of two electrons and holes, in the quantum dot results in the emission of a pair of photons at the energy of the biexciton and exciton transitions. The biexciton state was, in fact, proposed as a possible source of polarisation-entangled photons in 2000 by Benson et al. [3] as it consists of two polarisation-correlated decay paths which could potentially be indistinguishable. The condition of indistinguishability is fundamental to the generation of entangled photons and is, in general, not true of the two decay paths from the biexciton state in a quantum dot; physical anisotropy causes the intermediate exciton states to hybridise and separate in energy providing ‘which-path’ information about the route taken through the biexciton decay. We demonstrate how the splitting between the intermediate exciton states in a single InAs quantum dot can be controlled by growth [4], rapid thermal annealing [5] and the application of an external magnetic field [6]. Each of these three techniques can be used to make the intermediate exciton states degenerate allowing the biexciton decay to produce singe pairs of entangled photons triggered by short laser pulses [7,8]. Entangled photon pair sources are essential for applications such as entanglement based quantum key distribution, and optical quantum computing. For these applications it is important that no more than one entangled photon pair is generated in a cycle, a requirement met by our quantum dot source which is not possible with traditional methods for generating entangled pairs of photons. Entanglement also enables quantum interferometry and metrology, the basis of image resolution beyond that possible with equivalent classical light. Biphoton interferometry using entangled emission from the biexciton decay reveals fringes with half the period of classical light [9], and less that that of the laser. In addition, interferometry suggests that this type of entangled light source is not limited by decoherence, we fine the biphoton is surprising robust against dephasing, in stark contrast to the devastating effect of decoherence upon single photons emitted by similar structures.
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.
For scalable applications of optical quantum information it is desirable to have a well controlled source of photons, producing single photons or entangled-pairs on-demand. The finite delay following decay of an exciton confined in a quantum dot makes them a good source of single photons, we demonstrate this, triggering the emission with a pulsed laser. Currently the most widely used techniques for generating entangled photon pairs are nonlinear optical processes, such as parametric down conversion, which produces a probabilistic number of pairs per excitation cycle. Such a source is of limited use in quantum information/processing applications where a regular stream of single entangled photon pairs is preferable. We produced such a triggered source from a semiconductor device for the first time, using the two-photon cascade from a biexciton confined in a single quantum dot. We demonstrate a fidelity of 70% for the emission from the biexciton cascade to the expected bell state. Single quantum dots could prove to be the first robust and compact triggered source of entangled photons.
Emitters based on semiconductor quantum dots are promising sources for both single photons and pairs of polarization-entangled photons. Typically, single photons are generated through a photon emission event bringing the electronic system from a single-exciton state back to the ground state. In the case of entangled photons two photons are generated through a cascaded emission from the biexciton to either one of the single-exciton states and then back to the ground state. Alternatively, emission of two photons can also be achieved through a higher-order two-photon process bringing the quantum dot directly from the biexciton state (through a virtual intermediate state) back to the ground state. Here we discuss in particular how this two-photon process can lead to certain conceptual advantages in both the generation of polarization-entangled photon pairs and generation of single photons.