Dual frequency comb photon echo spectroscopy

Dual frequency comb (DFC) nonlinear spectroscopy is an emerging technique that can be used to study a variety of molecular nonlinear responses by exploiting the automatic pulse-to-pulse time delay scanning and fast data acquisition characteristics of the DFC techniques. Here, we propose a DFC-based photon echo spectroscopy (DFC-PES), where two optical frequency comb lasers have slightly different repetition rates and are also allowed to have different carrier frequencies. We first demonstrate our theoretical approach for DFC linear spectroscopy. Then, the signals expected from the proposed DFC-PES are theoretically calculated. The slight offset in the pulse repetition rates enables asynchronous optical sampling and automatic scanning of the time intervals between different field–matter interaction events, making frequency tuning unnecessary. Analytic expression of the third-order photon echo signal is demonstrated in two frequency dimensions for a simple two-level model system. The signal has a well-defined and simple connection to the underlying third-order response function and exhibits the expected down-conversion features from the optical frequency into the radio frequency region with a down-conversion factor that is experimentally controllable.