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We theoretically propose a multidimensional high-harmonic echo spectroscopytechnique which utilizes strong optical fields to resolve coherent electrondynamics spanning an energy range of multiple electron Volts. Using ourrecently developed semi-perturbative approach, we can describe the coherentvalence electron dynamics driven by a sequence of phase-matched and wellseparated short few-cycle strong infrared laser pulses. The recombination oftunnel-ionized electrons by each pulse coherently populates the valence statesof a molecule, which allows for a direct observation of its dynamics via thehigh harmonic echo signal. The broad bandwidth of the effective dipole betweenvalence states originated from the strong-field excitation results innontrivial ultra-delayed partial rephasing echo, which is not observed instandard 2D optical spectroscopic techniques. We demonstrate the results ofsimulations for the anionic molecular system and show that the ultrafastvalence electron dynamics can be well captured with femtosecond resolution.

Multidimensional high-harmonic echo spectroscopy: resolving coherent electron dynamics in the EUV regime