Electron Beam Driven Generation of Frequency-Tunable Isolated Relativistic Subcycle Pulses

Controlling the way light interacts with material excitations is at the heart of cavity quantum electrodynamics (QED). In the strong-coupling regime, quantum emitters in a microresonator absorb and spontaneously re-emit a photon many times before dissipation becomes effective, giving rise to mixed light-matter eigenmodes. Recent experiments in semiconductor microcavities reached a new limit of ultrastrong coupling, where photon exchange occurs on timescales comparable to the oscillation period of light. In this limit, ultrafast modulation of the coupling strength has been suggested to lead to unconventional QED phenomena. Although sophisticated light-matter coupling has been achieved in all three spatial dimensions, control in the fourth dimension, time, is little developed. Here we use a quantum-well waveguide structure to optically tune light-matter interaction from weak to ultrastrong and turn on maximum coupling within less than one cycle of light. In this regime, a class of extremely non-adiabatic phenomena becomes observable. In particular, we directly monitor how a coherent photon population converts to cavity polaritons during abrupt switching. This system forms a promising laboratory in which to study novel sub-cycle QED effects and represents an efficient room-temperature switching device operating at unprecedented speed.

We demonstrated how the subcycle evolution of the electric field of light can be used to control the motion of bound electrons. Results are presented for the dissociative ionization of deuterium molecules (D2 --> D+ + D), where asymmetric ejection of the ionic fragment reveals that light-driven intramolecular electronic motion before dissociation localizes the electron on one of the two D+ ions in a controlled way. The results extend subfemtosecond electron control to molecules and provide evidence of its usefulness in controlling reaction dynamics.