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Attosecond-Stable Two-Dimensional Spectroscopy by a Sagnac-Based Modulating System and a Sub-4-fs Continuum Source
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Attosecond-Stable Two-Dimensional Spectroscopy by a Sagnac-Based Modulating System and a Sub-4-fs Continuum Source

Wei-Chung Feng, Bo-Han Chen, Chih-Hsuan Lu, Howe-Siang Tan, Shang-Da Yang 和 Kai Chen
Laser & photonics reviews
09/09/2026
Web of Science ID: WOS:001870333200001

摘要

Optics Physical Sciences Physics Physics, Applied Physics, Condensed Matter Science & Technology
We present a two-dimensional electronic spectroscopy (2DES) platform driven by a Coherent Loop-based Integrated Modulating and Beamsplitting System (CLIMBS). Combined with an octave-spanning multiple-plate continuum (MPC) source, the system enables ultrabroadband, phase-coherent measurements with attosecond-level delay precision. Its Sagnac-inspired, nearly common-path geometry provides excellent long-term phase stability without active feedback while eliminating beam walk-off during delay scans. Delay calibration using spectrally resolved interferometric fringes confirmed precise, linear coherence-time control. The MPC source generates 550-980 nm excitation pulses compressed to 3.7 fs, enabling simultaneous excitation of widely separated electronic and vibronic transitions with high temporal and spectral resolution, and supporting distortion-free measurements of ground-state bleaching, stimulated emission, excited-state absorption, and vibronic cross peaks. The system's performance was evaluated using chlorophyll a in methanol, where the excitation bandwidth fully covers the and bands, enabling distortion-free 2DES measurements across the electronic manifold. This simple and robust platform provides high-fidelity ultrabroadband 2DES for multidimensional spectroscopy.

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https://doi.org/10.1002/lpor.71847檢視
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