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Single Molecules

Single Nanoobjects as Triggered Single Photons Sources

Brahim Lounis

Published Dec 1, 2001• 0 citations
Publisher

Abstract

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.

DOI
10.1002/1438-5171(200112)2:4<289::aid-simo289>3.0.co;2-m

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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.
The linear Stark effect on a single molecule allows us to sweep its frequency through resonance with a fixed laser frequency by applying a sinusoidal RF voltage on two electrodes. If the conditions of adiabatic following are fulfilled, we can prepare the excited molecular state with near certainty. Spontaneous emission from this state gives rise to a single photon. With our current experimental conditions, up to 75% of the sweeps lead to the emission of a single photon. Since the adiabatic passage is done on command, the molecule performs as a high rate source of triggered photons. The experimental results are in quantitative agreement with quantum Monte Carlo simulations.
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 deterministic "on demand" source of single photons is a basic building block for linear quantum computation \cite{linear}, quantum cryptography \cite{crypto}, quantum teleportation \cite{teleport}, and quantum networks \cite{network}. In all these applications, quantum interference between two single-photon pulses on a symmetric beam splitter has been exploited \cite{review}, which imposes stringent requirement for the implemented single photons to be indistinguishable in all degrees of freedom, including their frequencies, spectral widths, pulse shapes, and polarizations. To generate single photons one requires a pumping mechanism to excite a "two-level emitter" and an efficient channeling of the subsequently emitted photons. The efficiency of the source can be enhanced by coupling the emitter to the waveguide \cite{manga} or a microcavity mode \cite{cklaw}. However, hitherto the solid-state single photon sources realized by using a quantum dot coupled with a microcavity rely on incoherent pumping of excitons, which leads to problems with timing jitter \cite{kiraz}, leading to a trade off between efficiency and indistinguishability. Here we introduce a means to realize a highly efficient solid state source of indistinguishable single photons using cavity-assisted adiabatic Raman passage in a single quantum dot - cavity system. We demonstrate pulse-triggered single photons with 100% efficiency and >90>90>90% indistinguishability using currently available experimental parameters.
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.
Though QD arrays have initially been mostly studied in an attempt to improve semiconductor lasers, much attention has been recently devoted to the revolutionary prospects opened by the unique properties of single QDs. These artificial atoms allow to mimic in solid-state systems some of the quantum optics experiments performed on atoms since the early 80’s. Recent demonstrations of coherent control experiments on QDs illustrate this fruitful analogy [10]. We will focus here our discussion on the impact of QDs on two other fields, solid-state cavity quantum electrodynamics (CQED) and the generation of quantum states of light. A single QD can be used to emit triggered single photon pulses and photon pairs, whereas its narrow emission spectrum permits to implement microcavities very efficiently to tailor its emission properties. By combining both kind of effects, it is possible to control simultaneously the number of emitted photons as well as their quantum state and to build a solid-state singlemode source of single photons (singlemode S4P) as proposed [11] and demonstrated recently by our group [12]. This novel device represents the ultimate step in a field which has been extremely active in the last 15 years, spontaneous emission (SE) control in optoelectronic devices using confined electronic and/or photonic systems [13]. Before reviewing the development of this single mode S4P, based on a single QD in a pillar microcavity, we will briefly discuss its potential applications in the field of quantum information processing and quantum communications (QIPC).