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Single Molecules

Single Photon Light Sources

Karl Otto Greulich, E. Thiel

Published Mar 1, 2001• 13 citations
Publisher

Abstract

In the past, generation of single photons for subsequent use in physical or physicochemical experiments was difficult. In the last few years the situation has changed dramatically. Now, such sources based on a number of different techniques are available. Two of them produce antibunching photons by controlled recombination of electrons and holes in semiconductor heterojunctions. A second type of source is based on indium-arsenide quantum dots in high Q factor microcavities. Two further sources use single dibenz-anthanthrene or single terrylene molecules. While all but one sources have to be operated at temperatures close to zero Kelvin, the terrylene source works at room temperature and provides up to 10 billion photons before photodecay, i.e. it can be operated for hours. When the latter is operated at zero Kelvin, it is even more stable and can be used in a microscope to generate complete images. The present review compares and summarizes properties of these single optical photon sources and, in addition, tries to present an argument, why single photons cannot be particle like objects but must have a spatial extension of at least several tens of nanometers.

DOI
10.1002/1438-5171(200103)2:1<5::aid-simo5>3.0.co;2-9

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In the past, generation of single photons for subsequent use in physical or physicochemical experiments was difficult. In the last few years the situation has changed dramatically. Now, such sources based on a number of different techniques are available. Two of them produce antibunching photons by controlled recombination of electrons and holes in semiconductor heterojunctions. A second type of source is based on indium-arsenide quantum dots in high Q factor microcavities. Two further sources use single dibenz-anthanthrene or single terrylene molecules. While all but one sources have to be operated at temperatures close to zero Kelvin, the terrylene source works at room temperature and provides up to 10 billion photons before photodecay, i.e. it can be operated for hours. When the latter is operated at zero Kelvin, it is even more stable and can be used in a microscope to generate complete images. The present review compares and summarizes properties of these single optical photon sources and, in addition, tries to present an argument, why single photons cannot be particle like objects but must have a spatial extension of at least several tens of nanometers.
The concept of the photon , central to Einstein's explanation of the photoelectric effect, is exactly 100 years old. Yet, while photons have been detected individually for more than 50 years, devices producing individual photons on demand have only appeared in the last few years. New concepts for single-photon sources, or 'photon guns', have originated from recent progress in the optical detection, characterization and manipulation of single quantum objects. Single emitters usually deliver photons one at a time. This so-called antibunching of emitted photons can arise from various mechanisms, but ensures that the probability of obtaining two or more photons at the same time remains negligible. We briefly recall basic concepts in quantum optics and discuss potential applications of single-photon states to optical processing of quantum information: cryptography, computing and communication. A photon gun's properties are significantly improved by coupling it to a resonant cavity mode, either in the Purcell or strong-coupling regimes. We briefly recall early production of single photons with atomic beams, and the operation principles of macroscopic parametric sources, which are used in an overwhelming majority of quantum-optical experiments. We then review the photophysical and spectroscopic properties and compare the advantages and weaknesses of various single nanometre-scale objects used as single-photon sources: atoms or ions in the gas phase and, in condensed matter, organic molecules, defect centres, semiconductor nanocrystals and heterostructures. As new generations of sources are developed, coupling to cavities and nano-fabrication techniques lead to improved characteristics, delivery rates and spectral ranges. Judging from the brisk pace of recent progress, we expect single photons to soon proceed from demonstrations to applications and to bring with them the first practical uses of quantum information.
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.
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.
Single molecules in suitable host crystals have been demonstrated to be useful single-photon emitters both at liquid-helium temperatures and at room temperature. The low-temperature source achieved controllable emission of single photons from a single terrylene molecule in p -terphenyl by an adiabatic rapid passage technique. In contrast with almost all other single-molecule systems, terrylene single molecules show extremely high photostability under continuous, high-intensity irradiation. A room-temperature source utilizing this material has been demonstrated, in which fast pumping into vibrational sidebands of the electronically excited state achieved efficient inversion of the emissive level. This source yielded a single-photon emission probability p (1) of 0.86 at a detected count rate near 300 000 photons s −1 , with very small probability of emission of more than one photon. Thus, single molecules in solids can be considered as contenders for applications of single-photon sources such as quantum key distribution.
Quantum light and in particular single photons have become essential resources for a growing number of quantum applications including quantum computing, quantum key distribution and quantum metrology. Solid-state atomlike systems such as semiconductor quantum dots and color defects in crystals have become the hallmark of highly pure single photon emitters in the past two decades. A particular interest has been developed in nanocrystal quantum dots (NQDs) and color centers in diamond as potential compact room-temperature emitters. There are however several challenges that inhibit the use of such sources in current technologies including low photon extraction efficiency, low emission rates and relatively low single photon purities. In this work we will review our efforts in overcoming these technical difficulties using several complementary methods including designing several nanoantenna devices that enhance the directionality and emission rate of the nanoemitter. In addition, we developed several temporal heralding techniques to overcome the hurdle of low single photon purity in NQDs in an effort to produce a highly pure, bright and efficient single photon source on-chip.