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APL Photonics

Time–frequency mode structure study of ultrafast two-photon quantum state with two-color dual-comb-based optical sampling

Prasad Koviri, Takahisa Kuwana, Hajime Komori, Masahiro Ishizeki, Takashi Kato, Akifumi Asahara, T. R. Schibli, Ryōsuke Shimizu, Kaoru Minoshima

Published May 1, 2025• 2 citations
Publisher

Abstract

Quantum correlations of ultrafast quantum optical states in the time–frequency domain manifest prominently on femtosecond time scales, an elusive challenging regime. We develop a new method to probe the time–frequency mode structure of ultrafast two-photon states utilizing dual-comb-based asynchronously overlapping pulses with single-photon frequency upconversion through femtosecond optical sampling. This method enables quick, highly precise joint temporal intensity measurements over a broad temporal dynamic range with only a single linear scanning stage. We demonstrate full characterization of time–frequency entangled two-photon states in both time and frequency domains. We quantified the time–frequency mode structure in both time and frequency domains through Schmidt decomposition, resulting in temporal and spectral purities of 87.7% and 76.9%, respectively, for heralded single-photons without any spectral filtering. Furthermore, through the simple control of pump spectral bandwidth, we demonstrate the ability to tailor time–frequency entanglement, verifying the two-dimensional Fourier duality. This method paves the way for a substantial upgrade to ultrafast quantum optical techniques, enabling a rapid, detailed, and multi-dimensional characterization of entangled states with potential applications in quantum metrology and photon-deficient fluorescence imaging.

DOI
10.1063/5.0253108

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Quantum correlations of ultrafast quantum optical states in the time–frequency domain manifest prominently on femtosecond time scales, an elusive challenging regime. We develop a new method to probe the time–frequency mode structure of ultrafast two-photon states utilizing dual-comb-based asynchronously overlapping pulses with single-photon frequency upconversion through femtosecond optical sampling. This method enables quick, highly precise joint temporal intensity measurements over a broad temporal dynamic range with only a single linear scanning stage. We demonstrate full characterization of time–frequency entangled two-photon states in both time and frequency domains. We quantified the time–frequency mode structure in both time and frequency domains through Schmidt decomposition, resulting in temporal and spectral purities of 87.7% and 76.9%, respectively, for heralded single-photons without any spectral filtering. Furthermore, through the simple control of pump spectral bandwidth, we demonstrate the ability to tailor time–frequency entanglement, verifying the two-dimensional Fourier duality. This method paves the way for a substantial upgrade to ultrafast quantum optical techniques, enabling a rapid, detailed, and multi-dimensional characterization of entangled states with potential applications in quantum metrology and photon-deficient fluorescence imaging.
Abstract We demonstrated an ultrafast time-resolved measurement method operating at the single-photon level and employing a two-color comb-based asynchronous optical sampling (ASOPS) setup. We harnessed the two-color ASOPS photon counting approach to achieve long-term averaging of the ultralow intensity signal with a synchronized optical trigger signal, which minimizes residual timing jitter between the two combs. A pulse-width limited picosecond cross-correlation signal was successfully obtained with a power level of <1 photon/pulse. This approach enables the thorough study of ultrafast time-resolved detection of entangled photon pairs, quantum mechanical correlations in the time-frequency domain and finds wide use in optical quantum technology.
The nonclassical light sources, such as frequency-time entangled photons, are anticipated to offer significant benefits for emerging quantum optical sensing or spectroscopic measurements and manifest on ultrafast time scales (sub-ps to fs). However, the constrained time resolution (ns to ps) of photon-counting detectors poses challenges in comprehensively characterizing their detailed properties on ultrafast time scales. Therefore, we present a novel asynchronous optical sampling (ASOPS) technique utilizing two-color optical frequency combs to demonstrate highly precise and sensitive ultrafast time-resolved cross-correlation measurements at the single-photon level. By employing photon counting statistics, this method successfully reconstructed the picosecond pulse width cross-correlation waveforms at extremely low power level (<1 photon per pulse), while effectively suppressing the residual temporal jitter between the two combs via optically triggered averaging using asynchronous optical sampling of combs. The use of repetition frequency stabilized distinct-wavelength pulses allowed for the effective suppression of strong background light from the pump through spectral filtering, achieving single-photon sensitivity. Subsequently, we parametrically down converted the frequency doubled light from the Er comb in the nonlinear ppKTP waveguide to generate quantum entangled photons at telecom band. A 9.04% Klyshko efficiency with a photon pair generation rate of 0.98 MHz/mW was obtained using heralding detection. Employing the established ASOPS technique to the generated photon pairs enabled the realization of ultrafast time-resolved and quantum mechanical correlation measurements. This paves the way for a versatile and comprehensive manipulation of quantum-entangled photon pairs in the time-domain, with potential applications in ultrafast optical quantum technology and ultrashort fluorescence measurements.
Precise manipulation of the time–frequency modes of entangled photons is crucial for future quantum science and technologies. Recently, the frequency-domain-quantum-optical-synthesis (FD-QOS) method was demonstrated by creating a superposition of different joint temporal amplitudes: those temporal distributions can be controlled by manipulating the joint spectral amplitude in 2D frequency space via a Fourier optical relation. This FD-QOS method provides an efficient, flexible, and easy-to-control way to precisely modulate the temporal distributions of the entangled photon in an ultrafast region. However, manipulation of only the temporal modes is not sufficient for various applications in quantum information, since spectral modulations are also needed on many occasions. Here, we present a proof-of-concept experiment of two-photon spectral modulation via temporal manipulation of a biphoton wave packet. This protocol, called time-domain-quantum-optical-synthesis (TD-QOS), is achieved by adjusting the relative phases between two joint temporal distributions. In addition, the two-photon joint spectral distributions are characterized by measuring the joint spectral intensities and Hong–Ou–Mandel interferences. The combination of FD-QOS and TD-QOS enables complete control over the biphoton states. Our work would further develop quantum technologies that rely on the time–frequency modes of entangled photons.
Frequency modes of light are one of the most promising platforms that provide access to high-dimensional quantum states amongst different photonic degrees of freedom capable of high-dimensionality, enabling robust, error-tolerant, and scalable quantum optical information systems. We demonstrate engineering of precisely controlled two-photon high-dimensional states entangled in frequency through time-domain Fourier optical synthesis. We generate and convert a continuous broadband frequency-entangled state into a large range of discrete frequency bins suitable for ITU standards, with spacings ranging from 12.5 GHz to 750 GHz, and observe spectral anticorrelations over 38 frequency bins, including intra-bin pure states at a 100 GHz bin spacing. We characterize the full quantum state dimensionality via Schmidt decomposition and observe lower bounds on the frequency-binned Hilbert-space dimensionalities of at least 289, formed by two entangled qudits with dimension 17. Furthermore, we demonstrate quantum nonlocality via frequency correlations in a transmission experiment over a campus-scale two-node fiber network. This work represents a crucial step towards building a versatile and relatively simple way of generating precisely controlled high-dimensional spectral qudits, with the potential of harnessing in wavelength-multiplexed quantum networks, high-dimensional information processing, and communication of quantum states specifically, and fiber-optic quantum remote sensing.
We demonstrate a technique for characterizing two-photon quantum states based on joint temporal correlation measurements using time-resolved single-photon detection by femtosecond up-conversion. We measure for the first time the joint temporal density of a two-photon entangled state, showing clearly the time anticorrelation of the coincident-frequency entangled photon pair generated by ultrafast spontaneous parametric down-conversion under extended phase-matching conditions. The new technique enables us to manipulate the frequency entanglement by varying the down-conversion pump bandwidth to produce a nearly unentangled two-photon state that is expected to yield a heralded single-photon state with a purity of 0.88. The time-domain correlation technique complements existing frequency-domain measurement methods for a more complete characterization of photonic entanglement.
Conventional optical synthesis, the manipulation of the phase and amplitude of spectral components to produce an optical pulse in different temporal modes, is revolutionizing ultrafast optical science and metrology. These technologies rely on the Fourier transform of light fields between time and frequency domains in one-dimensional space. However, within this treatment, it is impossible to incorporate the quantum correlation among photons. Here, we expand the Fourier synthesis into high-dimensional space to deal with the quantum correlation and carry out an experimental demonstration by manipulating the two-photon probability distribution of a biphoton in two-dimensional time and frequency space. As a potential application, we show the manipulation of a heralded single-photon wave packet, which is never explained by the conventional one-dimensional Fourier optics. Our approach opens up a new pathway to tailor the temporal characteristics of a photon wave packet with high-dimensional quantum-mechanical treatment. We anticipate that such high-dimensional treatment of light in time and frequency domains could bridge the research fields between quantum optics and ultrafast optical measurements.