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The Journal of Chemical Physics

Theory of antibunching of photon emission II

Kazuhiko Seki, Masanori Tachiya

Published May 19, 2009• 2 citations
Publisher

Abstract

Recently single photon emission has been observed for systems in which multiple excitons are generated by pulsed excitation. When fast pair annihilation of excitons takes place, finally a single exciton remains and single photon can be emitted. Its efficiency depends on the competition among pair annihilation, unimolecular nonradiative, and radiative processes. The efficiency of single photon emission is usually studied by measuring the correlation of emitted photons after pulsed excitation by the Hanbury-Brown and Twiss method. The photon correlation measured in this method is different from that calculated by taking into account all pairs of emitted photons, which was presented in a previous paper. We calculate the former rigorously for the first time in the case of multiple excitations and compare it with the latter. We also calculate correlation of arrival times of two photons by the Hanbury-Brown and Twiss method. These results should be useful for the analysis of the antibunching measurement by the Hanbury-Brown and Twiss method.

DOI
10.1063/1.3134117

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Recently single photon emission has been observed for systems in which multiple excitons are generated by pulsed excitation. When fast pair annihilation of excitons takes place, finally a single exciton remains and single photon can be emitted. Its efficiency depends on the competition among pair annihilation, unimolecular nonradiative, and radiative processes. The efficiency of single photon emission is usually studied by measuring the correlation of emitted photons after pulsed excitation by the Hanbury-Brown and Twiss method. The photon correlation measured in this method is different from that calculated by taking into account all pairs of emitted photons, which was presented in a previous paper. We calculate the former rigorously for the first time in the case of multiple excitations and compare it with the latter. We also calculate correlation of arrival times of two photons by the Hanbury-Brown and Twiss method. These results should be useful for the analysis of the antibunching measurement by the Hanbury-Brown and Twiss method.
Type-B InP∕GaInP quantum dots are expected to exhibit a type-II electronic structure. Evidence for this is provided by the variation in decay time of the ensemble as a function of excitation power density. Photon correlation measurements were subsequently performed on a single type-B InP∕GaInP quantum dot using a Hanbury-Brown and Twiss setup [Nature 178, 1447 (1956)]. Autocorrelation measurements were carried out under both continuous-wave and pulsed excitation conditions with single-photon emission observed in each case. The continuous-wave measurements display a pronounced antibunching dip at zero time delay while pulsed measurements enable the triggered generation of single photons on demand at a wavelength of approximately 750 nm.
The second-order photon correlation function g2(τ) is of great importance in quantum optics. g2(τ) is typically measured with the Hanbury Brown and Twiss (HBT) interferometer, which employs a pair of single-photon detectors and a dual-channel time acquisition module. Here, we demonstrate a new method to measure and extract g2(τ) with a standard single-photon avalanche photodiode (dead-time = 22 ns) and a single-channel time acquisition module. This is realized by shifting the coincidence counts of interest to a time window not affected by the dead-time and after-pulse of the detection system using a fiber-based delay line. The new scheme is verified by measuring g2(τ) from a single colloidal nanocrystal. Photon antibunching is unambiguously observed and agrees well with the result measured using the standard HBT setup. Our scheme simplifies the higher-order correlation technique and might be favored in cost-sensitive circumstances.
Photon statistics divides light sources into three different categories, characterized by bunched, antibunched, or uncorrelated photon arrival times. Single atoms, ions, molecules, or solid state emitters display antibunching of photons, while classical thermal sources exhibit photon bunching. Here we demonstrate a light source in free space, where the photon statistics depends on the direction of observation, undergoing a continuous crossover between photon bunching and antibunching. We employ two trapped ions, observe their fluorescence under continuous laser light excitation, and record spatially resolved the autocorrelation function g^{(2)}(τ) with a movable Hanbury Brown and Twiss detector. Varying the detector position we find a minimum value for antibunching, g^{(2)}(0)=0.60(5) and a maximum of g^{(2)}(0)=1.46(8) for bunching, demonstrating that this source radiates fundamentally different types of light alike. The observed variation of the autocorrelation function is understood in the Dicke model from which the observed maximum and minimum values can be modeled, taking independently measured experimental parameters into account.
The formation of protein complexes with other proteins and nucleic acids is critical to biological function. Although it is relatively easy to identify the components present in these complexes, it is often difficult to determine their exact stoichiometry and obtain information about the homogeneity of the sample from bulk measurements. We demonstrate the use of single molecule photon-pair correlation spectroscopy to distinguish between discrete numbers of molecules in biological complexes. Fluorescence photon antibunching is observed from a single molecule by employing time-correlated single photon counting in combination with a Hanbury-Brown and Twiss coincidence setup. In addition, pulsed laser excitation and time-tagged time-resolved data collection allow for the measurement of photon arrival times with nanosecond time resolution. The interphoton time distribution between consecutively arriving photons can be calculated and provides a measure of the second-order temporal correlation function. Analysis of this function yields an absolute measure of the number of molecules, N, present in a given complex. It is this ability to measure N that renders this technique powerful for determining stoichiometries in complex biological systems at the single molecule level. We investigate the counting efficiency and statistics of photon antibunching of specifically designed biological samples labeled with multiple copies of the same fluorescent dye and derive conclusions about its use in the analytical evaluation of complex biological samples.
The development of quantum-enhanced technologies requires single-photon sources, as well as methods for their characterization and verification. Here, we describe a methodology for measuring the correlation function of a single-photon source using an experimental setup that comprises a laser-excited fluorescence microscope equipped with a Hanbury Brown–Twiss intensity interferometer as one of the detection systems. Measurements of the response function of the device and the reference samples are performed. The second-order autocorrelation function of the exciton state of GaAs quantum dots in AlGaAs nanowires is obtained and reveals a single-photon emission.
We report the observation of antibunched emission from single self-assembled InAs quantum dots under various conditions. We have measured the correlation function of the photon emission pertaining to single emission lines from single quantum dots under continuous and pulsed laser excitation, as well as under continuous white light excitation. The measurements were performed under different excitation intensities at liquid helium temperatures on two samples with distinct structures. At higher temperatures (30 K), an antibunching dip was still observed. We have also observed antibunching on a second emission line in the quantum dot spectrum, attributed to the biexciton, demonstrating the possibility of generating photon pairs with a single quantum dot. Polarization correlations on the biexciton and exciton line were also measured in an attempt to generate entangled photon pairs.