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Communications in Physics

Measuring anti-bunching Effect from Single Dye Molecules and Single Quantum Dots

Nguyen Thi Thanh Bao, Dinh Van Trung, Dang Tuyet Phuong

Published Jul 19, 2016• 0 citations
Publisher

Abstract

Antibunching is a quantum effect demonstrating clearly the quantum nature of the radiation field. Its detection through measurements of the second order correlation function is a direct proof of the presence of single molecule or single nano particle. In this paper we present the experimental setup of the Hanbury Brown - Twiss interferometer and the measurement results of the antibunching effect from single Rhodamine B dye molecules and single CdTe quantum dots in dilute solution. By fitting the second order correlation data, we derive a fluorescence lifetime of approximately 2 ns for Rhodamine B and 45 ns for CdTe quantum dots. Our results demonstrate an alternative way for determining the fluorescence lifetime using the antibunching effect.

DOI
10.15625/0868-3166/26/1/7806

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Antibunching is a quantum effect demonstrating clearly the quantum nature of the radiation field. Its detection through measurements of the second order correlation function is a direct proof of the presence of single molecule or single nano particle. In this paper we present the experimental setup of the Hanbury Brown - Twiss interferometer and the measurement results of the antibunching effect from single Rhodamine B dye molecules and single CdTe quantum dots in dilute solution. By fitting the second order correlation data, we derive a fluorescence lifetime of approximately 2 ns for Rhodamine B and 45 ns for CdTe quantum dots. Our results demonstrate an alternative way for determining the fluorescence lifetime using the antibunching effect.
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.
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.
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Photon anti-bunching, which is characterized by the second-order temporal coherence function g(2)(0) < g(2)(τ), has previously been measured using single-photon counting methods. We experimentally demonstrate a homodyne detection technique for measuring the second-order coherence g(2)(τ) of quantum states of light at sideband frequencies. Our scheme is based on the original Hanbury-Brown-Twiss (HBT) intensity interferometer, but instead replaces all use of photon counters with homodyne detection in each arm (see Fig. 1). The second-order coherence, g(2)(τ), is obtained from a set of quadrature amplitude measurements.
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 use of a Hanbury-Brown Twiss apparatus to measure auto- and cross-correlations from pairs of dye molecules tethered to single strands of DNA and coupled by Fluorescence Resonance Energy Transfer (FRET). We observe non-classical photon anti-bunching, and we note that certain features of the observed correlations most likely arise from conformational fluctuations in the biomolecular substrate. These techniques should provide experimental access to molecular dynamics at nanosecond (and longer) timescales.