Attosecond and sub-attosecond pulses in the deep-ultraviolet (DUV), vacuum-ultraviolet (VUV), and soft-x-ray regimes provide direct access to electron dynamics in different electronic shells on their natural timescales. Despite rapid experimental progress, the temporal characterization of broadband VUV pulses and ultrabroadband soft-x-ray attosecond pulses remains a central and largely unresolved challenge. Here, we introduce a single-shot pulse-reconstruction framework that, for the first time, combines direct numerical solutions of the three-dimensional time-dependent Schrödinger equation (3D-TDSE) with data-driven optimization. By abandoning semi-analytical response models and instead employing full electron dynamics as the forward mapping, the reconstruction signal acquires substantially enhanced sensitivity to ultrabroadband waveforms, even in the presence of strong Coulomb and strong-field effects. We demonstrate accurate and noise-robust reconstructions of isolated attosecond pulses, attosecond pulse trains, and femtosecond-to-attosecond VUV pulses in regimes where conventional strong-field-approximation (SFA) or perturbative model-based approaches fail. Our work establishes a fundamentally different paradigm for attosecond pulse metrology, enabling reliable single-shot characterization across the VUV and soft-x-ray spectral regions.

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• High-order harmonic generation
• Metrology
• Ultrafast optics
• Ultrafast phenomena
• Attosecond laser irradiation
• First-principles calculations
• Optical techniques
• X-ray techniques