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arXiv:2510.01836

Hybrid biphoton spectrometer for time-resolved quantum spectroscopy across visible and near-infrared regions

Ozora Iso, Onoda, Koya, Fairbairn, Nicola J., Masahiro Yabuno, Hirotaka Terai, Shigehito Miki, Ryōsuke Shimizu

Published Oct 2, 2025• 0 citations
arXivHTMLPDF

Abstract

Joint spectral measurements are a powerful tool for characterising biphoton spectral correlation, which is crucial for quantum information and communication technologies. In these applications, highly pure biphoton states are essential in any time- and frequency-mode, often obviating the need for time-resolved measurements. Conversely, spectroscopy utilising entangled photon pairs is gaining significant attention for its ability to unveil molecular dynamics, a field that critically demands time-resolved capabilities. Here, we introduce a methodology for capturing a biphoton spectrum that comprises visible and near-infrared photons, resulting in a highly non-degenerate joint spectrum. Our system employs two non-scanning spectrographs: a fibre spectrometer for near-infrared photons and a delay-line-anode single-photon imager for visible photons. We successfully measure the joint spectral intensity by leveraging a time-tagging acquisition strategy. Furthermore, our approach uniquely enables time-resolved joint spectral measurements with respect to the laser synchronisation against the hundreds-of-picosecond instrument response function. Our methodology could advance heralded fluorescence spectroscopy using biphoton sources to investigate temporal dynamics of complex biological, chemical, and physical systems.

DOI
10.48550/arxiv.2510.01836

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Joint spectral measurements are a powerful tool for characterising biphoton spectral correlation, which is crucial for quantum information and communication technologies. In these applications, highly pure biphoton states are essential in any time- and frequency-mode, often obviating the need for time-resolved measurements. Conversely, spectroscopy utilising entangled photon pairs is gaining significant attention for its ability to unveil molecular dynamics, a field that critically demands time-resolved capabilities. Here, we introduce a methodology for capturing a biphoton spectrum that comprises visible and near-infrared photons, resulting in a highly non-degenerate joint spectrum. Our system employs two non-scanning spectrographs: a fibre spectrometer for near-infrared photons and a delay-line-anode single-photon imager for visible photons. We successfully measure the joint spectral intensity by leveraging a time-tagging acquisition strategy. Furthermore, our approach uniquely enables time-resolved joint spectral measurements with respect to the laser synchronisation against the hundreds-of-picosecond instrument response function. Our methodology could advance heralded fluorescence spectroscopy using biphoton sources to investigate temporal dynamics of complex biological, chemical, and physical systems.
Distinguishing photon arrival time and position is crucial for advancing quantum technology. However, capturing spatial and temporal information efficiently remains challenging. Here, we present a novel photon detection technique to achieve a significantly more efficient measurement of frequency-entangled biphoton than conventional photon detectors. We utilize a delay-line-anode single-photon detector (DLD), which consists of a position-sensitive delay-line anode sensor behind a microchannel plate. Biphotons are obtained from the decay of biexcitons in the copper chloride semiconductor crystal. Two DLDs are coupled with a grating spectrometer exit to measure the joint spectral distributions of the biphoton. The resulting non-scanning process requires only a few minutes to obtain a temporally and spectrally resolved image, much quicker than the scanning biphoton frequency measurements such as monochromator or Fourier spectroscopy. Our technique paves the way for all experiments in multi-mode quantum science requiring coincidence measurement.
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Quantum physics holds promise to revolutionise a number of technologies by enabling performance beyond what is feasible with classical resources, such as secure communications, precision measurement and high-speed simulation and computation. To realise this, quantum information must be encoded into one of the physical degrees of freedom of light. The time-frequency (TF) domain provides a infinite-dimensional space which is naturally compatible with integrated optical platforms. Additionally, future quantum networks will require coherent coupling of quantum systems that do not necessarily exhibit TF mode overlap. The ability to generate, coherently control and measure a variety of TF states of quantum light is therefore a necessary step towards implementing optical quantum technologies. Developing the building blocks for future optical quantum applications calls for an assortment of methods for measuring the properties of TF states of quantum light. Whilst much progress has been made towards this goal recently, deficiencies with existing methods remain. Efficient spectrally-resolved detection away from the telecoms wavelength range and a robust approach to single-photon state characterisation that is sensitive to the spectral phase have so far proven challenging. Additionally, accessing quantum advantages requires measurements that are sensitive to the nonclassical correlations that can exist between separate subsystems. However, until now a flexible approach to determining the full quantum state of systems of multiple time/frequency entangled photons has been lacking. Here we develop a toolbox of techniques for the measurement of TF quantum states of light for few-photon systems, and apply these to the task of precision measurement. Firstly, we propose, construct and demonstrate efficient single-photon spectrometers based on dispersive time-to-frequency mapping, using chirped fibre Bragg gratings to apply the necessary group delay dispersion. We use two such devices operating in coincidence to realise a full phase-sensitive reconstruction of the TF state of a single photon, by spectrally resolving the output of a nonclassical interference process with an external reference. We also demonstrate a complementary, optical reference-free method. This characterisation tool, an implementation of electro-optic spectral shearing interferometry with coincident spectrally-resolved single-photon detection, melds techniques from ultrafast metrology and quantum optics. We proceed to demonstrate the flexibility of this device by reconstructing a wide range of test pulses generated with a pulse shaper. By implementing this technique in conjunction with spectrally-resolved detection of a second photon, we realise complete characterisation of the TF wave function of a spectrally-entangled broadband photon pair. This method is robust to a wide range of inputs and is generalisable to spectrally mixed states and across a wide range of wavelengths, including to spectrally non-degenerate photon pairs. To demonstrate, we generate an entangled photon pair with controllable TF entanglement and perform a full reconstruction. Lastly, we present a new technique for using TF entangled photon pairs to realise quantum-enhanced measurement of a time delay in a quantum channel in the presence of environmental noise. This scheme is based on entanglement-enhanced rejection of background light. A simple experiment demonstrating the feasibility of such a measurement is presented.
Recent advances in techniques for generating quantum light have stimulated research on novel spectroscopic measurements using quantum entangled photons. One such spectroscopy technique utilizes non-classical correlations among entangled photons to enable measurements with enhanced sensitivity and selectivity. Here, we investigate the spectroscopic measurement utilizing entangled three photons. In this measurement, time-resolved entangled photon spectroscopy with monochromatic pumping [A. Ishizaki, J. Chem. Phys. 153, 051102 (2020)] is integrated with the frequency-dispersed two-photon counting technique, which suppresses undesired accidental photon counts in the detector and thus allows one to separate the weak desired signal. This time-resolved frequency-dispersed two-photon counting signal, which is a function of two frequencies, is shown to provide the same information as that of coherent two-dimensional optical spectra. The spectral distribution of the phase-matching function works as a frequency filter to selectively resolve a specific region of the two-dimensional spectra, whereas the excited-state dynamics under investigation are temporally resolved in the time region longer than the entanglement time. The signal is not subject to Fourier limitations on the joint temporal and spectral resolution, and therefore, it is expected to be useful for investigating complex molecular systems in which multiple electronic states are present within a narrow energy range.
The spectral distribution of photon pairs produced by spontaneous parametric downconversion (SPDC) is one of the most exploited degrees of freedom in multiphoton experiments. Consequently, the characterization of such correlations is, without a doubt, a task of utmost importance. Common methods for measuring the joint spectral intensity (JSI) of correlated photon pairs often exhibit several drawbacks, such as the requirement for a bright source to offset high losses or the need for two-dimensional measurements, which can lead to prolonged acquisition times. In this work, we experimentally demonstrate a technique that allows for the reconstruction of the JSI from a single interferometric measurement, thus reducing the dimensionality of the problem. The reconstructed JSIs show good agreement with those obtained directly through a fiber spectrometer, confirming the effectiveness of our approach. This technique significantly enhances the efficiency of JSI characterization, offering a resource-efficient method for quantum state characterization in SPDC-based experiments.