Ultrafast Broadband Strong-Field Tunnelling in Asymmetric Nanogaps for Time-Resolved Nanoscopy

Abstract: Femtosecond-fast and nanometre-size pulses of electrons are emerging as unique probes for ultrafast dynamics at the nanoscale. Presently, such pulses are achievable only in highly sophisticated ultrafast electron microscopes or equally complex setups involving few-cycle-pulsed lasers with stable carrier-envelope phase (CEP) and nanotip probes. Here, we show that the generation of femtosecond pulses of nanoscale tunnelling electrons can be achieved in any ultrafast optical laboratory, using any (deep-UV to mid-IR) femtosecond laser in combination with photosensitive asymmetric nanogap (PAN) diodes fabricated via easy-to-scale adhesion lithography. The dominant mechanism producing tunnelling electrons in PANs is strong-field emission, which is easily achievable without CEP locking or external bias voltage. We employ PANs to demonstrate ultrafast nanoscopy of metal-halide perovskite quantum dots immobilised inside a 10-nm Al/Au nanogap and to characterise laser pulses across the entire optical region (266-6700 nm). Short electron pulses in PANs open the way towards scalable on-chip femtosecond electron measurements and novel design approaches for integrated ultrafast sensing nanodevices.