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arXiv:physics/0604180 · Optics Express

Photon-correlation Fourier spectroscopy

Xavier Brokmann, Moungi G. Bawendi, Laurent Coolen, Jean‐Pierre Hermier

Published Jan 1, 2006• 69 citations
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Abstract

We describe a method to probe the spectral fluctuations of a transition over broad ranges of frequencies and timescales with the high spectral resolution of Fourier spectroscopy, and a temporal resolution as high as the excited state lifetime, even in the limit of very low photocounting rates. The method derives from a simple relation between the fluorescence spectral dynamics of a single radi-ating dipole and its fluorescence intensity correlations at the outputs of a continuously scanning Michelson interferometer. These findings define an approach to investigate the fast fluorescence spectral dynamics of single molecules and other faint light sources beyond the time-resolution capabilities of standard spectroscopy experiments.

DOI
10.1364/oe.14.006333

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We describe a method to probe the spectral fluctuations of a transition over broad ranges of frequencies and timescales with the high spectral resolution of Fourier spectroscopy, and a temporal resolution as high as the excited state lifetime, even in the limit of very low photocounting rates. The method derives from a simple relation between the fluorescence spectral dynamics of a single radi-ating dipole and its fluorescence intensity correlations at the outputs of a continuously scanning Michelson interferometer. These findings define an approach to investigate the fast fluorescence spectral dynamics of single molecules and other faint light sources beyond the time-resolution capabilities of standard spectroscopy experiments.
The excited state population of single solid-state emitters is subjected to energy fluctuations around the equilibrium driven by the bath and relaxation through the emission of phonons or photons. Simultaneous measurement of the associated spectral dynamics requires a technique with a high spectral and temporal resolution with an additionally high temporal dynamic range. We propose a pulsed excitation-laser analog of photon-correlation Fourier spectroscopy (PCFS), which extracts the linewidth and spectral diffusion dynamics along the emission lifetime trajectory of the emitter, effectively discriminating spectral dynamics from relaxation and bath fluctuations. This lifetime-resolved PCFS correlates photon-pairs at the output arm of a Michelson interferometer in both their time-delay between laser-excitation and photon-detection T and the time-delay between two photons τ. We propose the utility of the technique for systems with changing relative contributions to the emission from multiple states, for example, quantum emitters exhibiting phonon-mediated exchange between different fine-structure states.
We show that the single emitter linewidth underlying a broadened ensemble emission spectrum can be extracted from correlations among the stochastic intensity fluctuations in the ensemble spectrum. Spectral correlations can be observed at high temporal and spectral resolutions with a cross-correlated pair of avalanche photodiodes placed at the outputs of a scanning Michelson interferometer. As illustrated with simulations in conjunction with Fluorescence Correlation Spectroscopy, our approach overcomes ensemble and temporal inhomogeneous broadening to provide single emitter linewidths, even for emitters under weak, continuous, broadband excitation.
Classical time-resolved optical spectroscopy experiments are performed using sequences of ultrashort light pulses, with photon fluxes incident on the sample which are many orders of magnitude higher than real-world conditions corresponding to sunlight illumination. Spectroscopy and microscopy schemes that use quantum states of light have been widely described theoretically with fewer experimental demonstrations that typically require very long measurements that can extend for hours or more. Here, we show that time-resolved spectroscopy with quantum light can be performed without compromising measurement time or wavelength tunability, recording a fluorescence lifetime trace in biological samples in less than a second with acceptable signal-to-noise ratio. Starting from spontaneous parametric down-conversion driven by a continuous-wave laser, we exploit the temporal correlation between randomly generated signal/idler pairs to obtain temporal resolution, and their spectral correlation to select the excitation frequency. We also add spectral resolution in detection, using a 'photon-efficient' Fourier transform approach which employs a common-path interferometer. We demonstrate the potential of this approach by resolving, at the single-photon level, excitation energy transfer cascades from LH2 to LH1 in the photosynthetic membrane and disentangling the lifetimes of two dyes in a mixture. Our results provide a new approach to ultrafast optical spectroscopy, where experiments are performed under illumination intensity conditions comparable to real-world sunlight illumination.
Classical time-resolved optical spectroscopy experiments are performed using sequences of ultrashort light pulses, with photon fluxes incident on the sample which are many orders of magnitude higher than real-world conditions corresponding to sunlight illumination. Here we overcome this paradigm by exploiting quantum correlations to perform time-resolved spectroscopy with entangled photons. Starting from spontaneous parametric down-conversion driven by a continuous-wave laser, we exploit the temporal entanglement between randomly generated signal/idler pairs to obtain temporal resolution, and their spectral entanglement to select the excitation frequency. We also add spectral resolution in detection, using a Fourier transform approach which employs a common-path interferometer. We demonstrate the potential of our entangled-photon streak camera by resolving, at the single-photon level, excitation energy transfer cascades from LH2 to LH1 in the photosynthetic membrane and disentangling the lifetimes of two dyes in a mixture. We show that time-resolved spectroscopy with quantum light can be performed without compromising measurement time, recording a fluorescence time trace in less than a minute even for samples with low quantum yield, which can be reduced to sub-second times with acceptable signal-to-noise ratio. Our results provide a new approach to ultrafast optical spectroscopy, where experiments are performed under conditions comparable to real-world sunlight illumination.
Light emission from solid-state quantum emitters is inherently prone to environmental decoherence, which results in a line broadening and in the deterioration of photon indistinguishability. Here we employ photon correlation Fourier spectroscopy (PCFS) to study the temporal evolution of such a broadening in two prominent systems: GaAs and In(Ga)As quantum dots. Differently from previous experiments, the emitters are driven with short laser pulses as required for the generation of high-purity single photons, the time scales we probe range from a few nanoseconds to milliseconds and, simultaneously, the spectral resolution we achieve can be as small as ∼ 2µeV. We find pronounced differences in the temporal evolution of different optical transition lines, which we attribute to differences in their homogeneous linewidth and sensitivity to charge noise. We analyze the effect of irradiation with additional white light, which reduces blinking at the cost of enhanced charge noise. Due to its robustness against experimental imperfections and its high temporal resolution and bandwidth, PCFS outperforms established spectroscopy techniques, such as Michelson interferometry. We discuss its practical implementation and the possibility to use it to estimate the indistinguishability of consecutively emitted single photons for applications in quantum communication and photonic-based quantum information processing.