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arXiv:2109.03715

Quantum Fourier transform spectroscopy of biexciton

Hiroya Seki, Kensuke Miyajima, Ryōsuke Shimizu

Published Sep 8, 2021• 0 citations
arXivHTMLPDF

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 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.

DOI
10.48550/arxiv.2109.03715

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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.
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.
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.
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