Ultrafast nano-focusing with full optical waveform control

Abstract: The spatial confinement and temporal control of an optical excitation on nanometer length scales and femtosecond time scales has been a long-standing challenge in optics. It would provide spectroscopic access to the elementary optical excitations in matter on their natural length and time scales and enable applications from ultrafast nano-opto-electronics to single molecule quantum coherent control. Previous approaches have largely focused on using surface plasmon polariton (SPP) resonant nanostructures or SPP waveguides to generate nanometer localized excitations. However, these implementations generally suffer from mode mismatch between the far-field propagating light and the near-field confinement. In addition, the spatial localization in itself may depend on the spectral phase and amplitude of the driving laser pulse thus limiting the degrees of freedom available to independently control the nano-optical waveform. Here we utilize femtosecond broadband SPP coupling, by laterally chirped fan gratings, onto the shaft of a monolithic noble metal tip, leading to adiabatic SPP compression and localization at the tip apex. In combination with spectral pulse shaping with feedback on the intrinsic nonlinear response of the tip apex, we demonstrate the continuous micro- to nano-scale self-similar mode matched transformation of the propagating femtosecond SPP field into a 20 nm spatially and 16 fs temporally confined light pulse at the tip apex. Furthermore, with the essentially wavelength and phase independent 3D focusing mechanism we show the generation of arbitrary optical waveforms nanofocused at the tip. This unique femtosecond nano-torch with high nano-scale power delivery in free space and full spectral and temporal control opens the door for the extension of the powerful nonlinear and ultrafast vibrational and electronic spectroscopies to the nanoscale.