Femtosecond spectroscopy with paired single photons: Emulating a double-slit experiment in the time-frequency domain
Year: 2025
Type: article
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.
Source: Science Advances
Authors: EunHo Hong, EunSeo Jang, JunWoo Kim
Institution: Chungbuk National University
Language: English
Subfield: Atomic and Molecular Physics, and Optics
Field: Physics and Astronomy
Domain: Physical Sciences
Open Access status: gold
Estimated APC paid: $4,500
OpenAlex ID: W4415285953