ArticleScience advances2025
Femtosecond spectroscopy with paired single photons: Emulating a double-slit experiment in the time-frequency domain.
Article in Science advances, 2025. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 2 papers.
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2 citing papers in PubMed.
- Quantum-Indeterminate Proton Positions in Ultrafast Excited-State Intramolecular Proton Transfer.The journal of physical chemistry letters · 2026Article
- Two-dimensional fluorescence spectroscopy with entangled photons and time- and frequency-resolved two-photon coincidence detection.Science advances · 2026Article
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3 authors.
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Abstract
Time-resolved spectroscopy has long served as a cornerstone technique for investigating the photophysics of materials. However, conventional methods based on intense optical pulses and ensemble measurements often fail to resolve quantum dynamics due to spectral overlap, coherent artifacts, and multiphoton effects. To overcome these limitations, single-photon transient stimulated emission (SP-TSE) has been proposed as a femtosecond spectroscopy technique using quantum light and detection principles. Here, we theoretically demonstrate frequency-resolved SP-TSE. Unlike semiclassical techniques, SP-TSE reveals a strong dependence of the time-resolved spectrum on the frequency-resolving method. With a tunable optical filter, the observed spectrum reflects a quantum double-slit interference in the time-frequency domain. In contrast, interferometric detection produces spectra resembling semiclassical results, but the signal emerges specifically from the second harmonic frequency window due to quantum interference. This framework provides insight into ultrafast quantum processes and suggests a foundation for future applications in quantum spectroscopy and technologies.
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