Ryosuke SHIMIZU (清水 亮介)

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.

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.

Ultrafast optical spectroscopy is a powerful technique for studying the dynamic processes of molecular systems in condensed phases. However, in molecular systems containing many dye molecules, the spectra can become crowded and difficult to interpret owing to the presence of multiple nonlinear optical contributions. In this work, we theoretically propose time-resolved spectroscopy based on the coincidence counting of two entangled photons generated via parametric down-conversion with a monochromatic laser. We demonstrate that the use of two-photon counting detection of entangled photon pairs enables the selective elimination of the excited-state absorption signal. This selective elimination cannot be realized with classical coherent light. We anticipate that the proposed spectroscopy will help simplify the spectral interpretation of complex molecular and material systems comprising multiple molecules.

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.

Hong-Ou-Mandel (HOM) interference of multi-mode frequency entangled states plays a crucial role in quantum metrology. However, as the number of modes increases, the HOM interference pattern becomes increasingly complex, making it challenging to comprehend intuitively. To overcome this problem, we present the theory and simulation of multi-mode-HOM interference (MM-HOMI) and compare it to multi-slit interference (MSI). We find that these two interferences have a strong mapping relationship and are determined by two factors: the envelope factor and the details factor. The envelope factor is contributed by the single-mode HOM interference (single-slit diffraction) for MM-HOMI (MSI). The details factor is given by sin (Nx)/sin (x) ([sin (Nv)/sin (v)]²) for MM-HOMI (MSI), where N is the mode (slit) number and x (v) is the phase spacing of two adjacent spectral modes (slits). As a potential application, we demonstrate that the square root of the maximal Fisher information in MM-HOMI increases linearly with the number of modes, indicating that MM-HOMI is a powerful tool for enhancing precision in time estimation. We also discuss multi-mode Mach-Zehnder interference, multi-mode NOON-state interference, and the extended Wiener-Khinchin theorem. This work may provide an intuitive understanding of MM-HOMI patterns and promote the application of MM-HOMI in quantum metrology.