Probing the Dynamics of Two-Level System Defect Ensembles via Broadband Cryogenic Transient Dielectric Spectroscopy

arXiv:2505.18263v4 Announce Type: replace-cross Abstract: Two-level system (TLS) defects in dielectrics are a major source of decoherence in superconducting circuits, yet their microscopic origin and distribution remain poorly understood. Existing circuit-QED probes access limited frequency ranges and mode volumes, restricting studies of isolated materials and interfaces. Here, we present Broadband Cryogenic Transient Dielectric Spectroscopy (BCTDS), a technique for probing TLS-hosting materials over a broad frequency range at cryogenic temperatures. Under strong finite-duration microwave excitation, the transient homodyne I-Q response exhibits coherent phase dynamics after the drive is turned off. Fourier analysis of the transient phase reveals characteristic V-shaped structures that move between cooldowns, consistent with thermocycling-induced changes in the local TLS defect environment that shift defect resonance frequencies. The transient response of BCTDS further enables estimation of susceptibility and two-time correlation functions of the TLS defect ensemble. The observed phase dynamics are qualitatively captured by a driven standard tunneling model containing only a few representative TLS defects. Despite its simplicity relative to the full experimental ensemble, the model reproduces the essential Floquet-dressed dynamics during the drive and generates post-pulse V-shaped structures and interference fringes consistent with the experimental data. The observed BCTDS response may reflect a crossover from localized TLS defect dynamics to a delocalized regime under strong driving, before being quenched into a transient regime that reflects the TLS defect resonance frequencies. Overall, BCTDS represents a potentially useful broadband, time-resolved wafer-level approach for probing TLS defects relevant to quantum technologies.