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Physical Review A

Quantum interferometric spectroscopy of a biexciton

Hiroya Seki, Kensuke Miyajima, Ryōsuke Shimizu

Published Dec 22, 2022• 6 citations
Publisher

Abstract

Fourier transform spectroscopy with classical interferometry corresponds to the measurement of a single-photon intensity spectrum from the viewpoint of the particle nature of light. In contrast, the Fourier transform of two-photon quantum interference patterns provides the intensity spectrum of the two photons as a function of the sum- or difference frequency of the constituent photons. This unique feature of quantum interferometric spectroscopy offers a different type of spectral information from the classical measurement and may prove useful for nonlinear spectroscopy with two-photon emission. Here, we report the experimental demonstration of two-photon quantum interference of biphotons emitted via biexcitons in the semiconductor CuCl. Besides applying Fourier transform to quantum interference patterns, we reconstruct the intensity spectrum of the biexciton luminescence in the two-photon sum- or difference frequency. We discuss the connection between the reconstructed spectra and exciton states in CuCl as well as the capability of quantum interferometry in solid-state spectroscopy.

DOI
10.1103/physreva.106.063716

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•Nov 15, 2011•0 citations
Fourier transform spectroscopy with classical interferometry corresponds to the measurement of a single-photon intensity spectrum from the viewpoint of the particle nature of light. In contrast, the Fourier transform of two-photon quantum interference patterns provides the intensity spectrum of the two photons as a function of the sum- or difference frequency of the constituent photons. This unique feature of quantum interferometric spectroscopy offers a different type of spectral information from the classical measurement and may prove useful for nonlinear spectroscopy with two-photon emission. Here, we report the experimental demonstration of two-photon quantum interference of biphotons emitted via biexcitons in the semiconductor CuCl. Besides applying Fourier transform to quantum interference patterns, we reconstruct the intensity spectrum of the biexciton luminescence in the two-photon sum- or difference frequency. We discuss the connection between the reconstructed spectra and exciton states in CuCl as well as the capability of quantum interferometry in solid-state spectroscopy.
Fourier transform spectroscopy with classical interferometry corresponds to the measurement of a single-photon intensity spectrum from the viewpoint of the particle nature of light. In contrast, the Fourier transform of two-photon quantum interference patterns provides the intensity spectrum of the two photons as a function of the sum or difference frequency of the constituent photons. This unique feature of quantum interferometric spectroscopy offers a different type of spectral information from the classical measurement and may prove useful for nonlinear spectroscopy with two-photon emission. Here, we report the first experimental demonstration of two-photon quantum interference of photon pairs emitted via biexcitons in the semiconductor CuCl. Besides applying Fourier transform to quantum interference patterns, we reconstruct the intensity spectrum of the biexciton luminescence in the two-photon sum or difference frequency. We discuss the connection between the reconstructed spectra and exciton states in CuCl as well as the capability of quantum interferometry in solid-state spectroscopy.
Abstract Two-photon excitation spectroscopy is a nonlinear technique that has gained rapidly in interest and significance for studying the complex energy-level structure and transition probabilities of materials. While the conventional spectroscopy based on tunable classical light has been long established, quantum light provides an alternative way towards excitation spectroscopy with potential advantages in temporal and spectral resolution, as well as reduced photon fluxes. By using a quantum Fourier transform that connects the sum-frequency intensity and N00N-state temporal interference, we present an approach for quantum interferometric two-photon excitation spectroscopy. Our proposed protocol overcomes the difficulties of engineering two-photon joint spectral intensities and fine-tuned absorption-frequency selection. These results may significantly facilitate the use of quantum interferometric spectroscopy for extracting the information about the electronic structure of the two-photon excited-state manifold of atoms or molecules without any requirement for precise and complicated scanning in the spectral domain. This may be particularly relevant for photon-sensitive biological and chemical samples.
We propose theoretically a quantum interferometer in which the NOON state interferometer is combined with the Hong-Ou-Mandel interferometer. With this interferometer, the temporal interference patterns associated with biphoton frequency sum and difference can be shown in different parts of a single interferogram. It is thus possible to simultaneously obtain the spectral correlation information of biphotons in both frequency sum and difference by taking the Fourier transform from such an interferogram. This provides a method for complete spectral characterization of an arbitrary two-photon state with exchange symmetry and might be useful in quantum Fourier-transform spectroscopy where direct spectral measurement is difficult. Furthermore, as it can realize the measurement of time intervals on three scales at the same time, we expect that it can provide a method in quantum metrology. Finally, we discuss another potential application of such an interferometer in the generation and characterization of high-dimensional and phase-controlled frequency entanglement.
The biexciton resonance in the absorption spectra of semiconductor quantum wells is analyzed with quantum-optical spectroscopy by projecting experimental pump-probe measurements into quantum-optical absorption spectra. More specifically, the measurements are converted into phase-space distributions using the cluster-expansion transformation. The quantum-optical responses can then be projected with full convergence, despite the unavoidable experimental noise. The calculations show that classical and quantum excitations produce significantly different results for the biexciton resonance. In particular, quantum-optical spectroscopy monitors the excitation-induced broadening of the biexciton resonance as a function of pump intensity much more sensitively than classical spectroscopy does.
Quantum interferences of entangled photons have engendered tremendous intriguing phenomena that lack any counterpart in classical physics. Hitherto, owing to the salient properties of quantum optics, quantum interference has been widely studied and provides useful tools that ultimately broaden the path towards ultra-sensitive quantum metrology, ranging from sub-shot-noise quantum sensing to high-resolution optical spectroscopy. In particular, quantum interferometric metrology is an essential requisite for extracting information about the structure and dynamics of photon-sensitive biological and chemical molecules. This article reviews the theoretical and experimental progress of this quantum interferometric metrology technology along with their advanced applications. The scope of this review includes Hong–Ou–Mandel interferometry with ultrahigh timing resolution, entanglement-assisted absorption spectroscopy based on a Fourier transform, and virtual-state spectroscopy using tunable energy-time entangled photons.
A well controlled, triggered source of entangled photons is desirable for many applications in quantum information processing. The two-photon cascade from a biexciton state, two electrons and holes, confined in a quantum dot can be such a source of polarisation-entangled photons provided the two decay paths from the biexciton carry no “which-path” information. In recent years many techniques have been employed to make the two optical decay paths from the biexciton state indistinguishable. A number of these techniques will be discussed and entangled-photon emission from a single quantum dot with a high fidelity in the expected Bell-state from the cascade will be demonstrated. This source of entangled photons allows optical interferometry beyond the limits imposed by the photon wavelength. Interference fringes of the entangled biphoton state reveals a periodicity half of that obtained with the single photon, and much less than that of the pump laser. High fringe visibility indicates that biphoton interference is less sensitive to decoherence than interference of two sequential single photons. The effect of the exciton fine-structure splitting on our entangled photon source will be shown. Surprisingly the entanglement is found to persist despite relatively large separations between the intermediate energy levels of up to 4µeV. Measurements demonstrate that entanglement of the photon pair is robust to the dephasing of the intermediate exciton state responsible for the first order coherence time of either single photon. We distinguish between the first-order coherence time, and a parameter defined as the cross-coherence time, this is illustrated in the figure.