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Physical Review Letters

Single-Mode Generation of Quantum Photon States by Excited Single Molecules in a Microcavity Trap

F. De Martini, Giovanni Di Giuseppe, Michele Marrocco

Published Feb 5, 1996• 168 citations
Publisher

Abstract

The active microcavity is adopted as an efficient source of nonclassical light. Using this device, excited with a mode-locked laser at a rate of 100 MHz, single photons are generated over a single field mode with a nonclassical sub-Poissonian distribution. Adiabatic recycling within a multistep Franck-Condon molecular optical-pumping mechanism, characterized by quantum efficiency close to 1, implies a pump self-regularization process leading to a striking $n$-squeezing effect. Replicating the basic single-atom excitation process a beam of quantum photon $|n〉$ states (Fock states) can be created. This represents a significant advance in the fields of basic quantum-mechanical investigation, quantum communication, and quantum cryptography.

DOI
10.1103/physrevlett.76.900

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Single Nanoobjects as Triggered Single Photons Sources

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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•Dec 1, 2001•0 citations

Generation of "triggered single photons" from a coherently-pumped quantum dot

Pradyumna K. Pathak, Stephen Hughes

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 $>90$% indistinguishability using currently available experimental parameters.

arXiv:0911.5673•Nov 30, 2009•0 citations
The active microcavity is adopted as an efficient source of nonclassical light. Using this device, excited with a mode-locked laser at a rate of 100 MHz, single photons are generated over a single field mode with a nonclassical sub-Poissonian distribution. Adiabatic recycling within a multistep Franck-Condon molecular optical-pumping mechanism, characterized by quantum efficiency close to 1, implies a pump self-regularization process leading to a striking nnn-squeezing effect. Replicating the basic single-atom excitation process a beam of quantum photon ∣n〉|n〉∣n〉 states (Fock states) can be created. This represents a significant advance in the fields of basic quantum-mechanical investigation, quantum communication, and quantum cryptography.
The active microcavity is adopted as an efficient source of non-classical light. By this device, excited by a mode-locked laser at a rate of 100 MHz, single-photons are generated over a single field mode with a nonclassical sub-poissonian distribution. The process of adiabatic recycling within a multi-step Franck-Condon molecular optical-pumping mechanism, characterized in our case by a quantum efficiency very close to one, implies a pump self-regularization process leading to a striking n-squeezing effect. By a replication of the basic single-atom excitation process a beam of quantum photon (Fock states) can be created. The new process represents a significant advance in the modern fields of basic quantum-mechanical investigation, quantum communication and quantum cryptography.
The active microcavity is adopted as an efficient source of non-classical light. By this device, excited by a mode-locked laser at a rate of 100 MHz, single photons are generated over a single field mode with a non-classical sub-Poissonian distribution. The process of adiabatic recycling within a multistep Franck–Condon molecular optical-pumping mechanism, characterized in our case by a quantum efficiency close to one, implies a pump self-regularization process leading to a striking n-squeezing effect. Moreover, the microactivity has been adopted as active beam splitter in a novel Hanbury-Brown–Twiss configuration for the radiation taking place over the two output mirrors. By a replication of the basic single-atom excitation process a beam of quantum photon |n〉 states (Fock states) can be created. The new process may represent a significant advance in the modern fields of basic quantum-mechanical investigation, quantum communication and quantum cryptography.
Some ultrafast phenomena occurring in an active microcavity have been investigated. This device can behave as an efficient source of non-classical light, when a small number of molecules inside are excited by a femtosecond laser.In this way single photon n > states are generated with anon-classical sub-Poissonian distribution. Multiple excitations of a larger number of molecules can give rise to collective phenomena because of the strong super-radiant ultrafast coupling within the transverse region of the microcavity electromagnetic field. This process has been experimentally studied by means of a high efficiency, single photon, femtosecond non-linear optical gate.
We present a scheme for the realization of a stationary source of nonclassical light, which approximates very well a continuous single-photon source. It consists of a single four-level atom trapped inside a high-finesse optical cavity and Raman coupled to a cavity mode. A selectivity mechanism, based on a field-dependent Stark shift of electronic levels, prevents the occupation of two or more photon states of the quantized mode being excited. The output light of such a source exhibits sub-Poissonian photon-number statistics and antibunching behavior.
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.
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.