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Single Molecules

The Emission of a Single Photon from a Single Atom or Molecule - An Experimenter's View

Karl Otto Greulich

Published Apr 1, 2002• 1 citation
Publisher

Abstract

Crucial experiments of physics, such as the quantum mechanical version of the double slit experiment, have so far not been performed with true single (antibunching) photons. Instead, attenuated classical light sources such as bulbs or lasers have been suggested to provide the photons in these experiments. Since attenuators do not change photon statistics, i.e. do not convert classical into non - classical light, reliable single photon beams cannot be generated on this way. Antibunching sources, for example single molecules, are required. Due to the lack of such sources in the past, some extrapolations from the many - photon case to the one photon case have remained speculative, for example the long wavetrain model for a single photon. Alternative hypotheses, elaborated by considering details of the emission of single photons by single molecules are equally probable. Arguments are presented which disfavour the wavetrain model and favour the short pulse as a model for a photon.

DOI
10.1002/1438-5171(200204)3:1<19::aid-simo19>3.0.co;2-z

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Single Molecules•Dec 1, 2001•0 citations
Crucial experiments of physics, such as the quantum mechanical version of the double slit experiment, have so far not been performed with true single (antibunching) photons. Instead, attenuated classical light sources such as bulbs or lasers have been suggested to provide the photons in these experiments. Since attenuators do not change photon statistics, i.e. do not convert classical into non - classical light, reliable single photon beams cannot be generated on this way. Antibunching sources, for example single molecules, are required. Due to the lack of such sources in the past, some extrapolations from the many - photon case to the one photon case have remained speculative, for example the long wavetrain model for a single photon. Alternative hypotheses, elaborated by considering details of the emission of single photons by single molecules are equally probable. Arguments are presented which disfavour the wavetrain model and favour the short pulse as a model for a photon.
Throughout the development and confirmation of the photon concept, "Gedankenexperiments" have been invoked where a light source is attenuated until "only one photon is in the apparatus." Such a statement requires, however, knowledge on details of the light generation process, which were not known until the advent of true single-photon light sources such as isolated single atoms or molecules. Here, starting from a two atom light source, it is shown that probably multi-atom or multi-molecule light sources do not generate, even not in small fractions, antibunching photons and that attenuation down to one photon per time unit is not reliably possible. Thus, one of the strongest arguments in favour of the existence of single "photons" in free space, the accumulation time argument, which discusses the absorption of a single photon by a single atom or molecule, becomes questionable.
Single molecule techniques improve our understanding of the photon and light. If the single photon double slit experiment is performed at the "single photon limit" of a multi-atom light source, faint light pulses with more than one photon hamper the interpretation. Single molecules, quantum dots or defect centres in crystals should be used as light source. "Single photon detectors" do not meet their promise-only "photon number resolving single photon detectors" do so. Particularly, the accumulation time argument, the only safe basis for the postulate of a strictly particle like photon, has so far not yet been verified.
Double slit experiments with true single photons are presently becoming reality. Thus one may speculate that the wave particle duality of light and photons can now be proven unequivocally. This was not the case with earlier experiments using attenuated multi-atom light sources. Here it is suggested that the few available experiments which indeed are using single photons can be explained in a comprehensible manner without invoking quantum mechanics and wave particle dualism. However, one has to give up the notion of an indivisible photon.
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 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.