Dual-mechanism tuned double-walled carbon nanotube cold-cathode for ultrafast electron emission

Cold-cathode ultrafast electron source is a key component for probing ultrafast dynamics behavior in materials, as well as developing high-frequency and high-power electromagnetic radiation devices. Developing large-current, high-brightness, and tunable ultrafast electron sources by leveraging the intrinsic properties of nanomaterials is significant. In this study, we report the in-situ assembly of a double-walled carbon nanotube (DWCNT) cold-cathode based on a tungsten (W) tip via nanotransfer manipulation within a scanning electron microscopy (SEM) chamber, enabled by electron-beam-induced carbon deposition. The resulting ultrafast electron emission exhibits excellent performance under dual-regime modulation by multiphoton photoemission (MPP) and optical field emission (OFE). Under co-excitation by 800 nm femtosecond laser pulses and a static electric field, the DWCNT cold-cathode demonstrates significantly enhanced emission in both regimes with a maximum peak current of ~ 65 A and a corresponding brightness of 4.98 × 10¹⁸ A·m⁻²·sr⁻¹·V⁻¹, and its optical excitation threshold reduces by an order of magnitude compared to the conventional metallic W tip cathode at equivalent emission current levels. Comprehensive material characterizations combined with density functional theory (DFT) calculations reveal that the semiconducting nature of the DWCNT emitter, along with its favorable electronic density of states and correspondingly lower effective work function, provides distinct advantages over metallic CNT and W for ultrafast electron emission. Furthermore, quantitative models are developed for both MPP- and OFE-dominated regimes, which elucidate polarization-dependent electron emission behavior and its underlying physical mechanisms. This work presents a promising semiconducting DWCNT cold-cathode for high-performance ultrafast electron sources, and provides a path for investigating ultrafast electron emission dynamics from multiple perspectives.