Multi-color quantum control for suppressing ground state coherences in two-dimensional electronic spectroscopy

Abstract

The measured multi-dimensional spectral response of different light harvesting complexes exhibits oscillatory features which suggest an underlying coherent energy transfer. However, making this inference rigorous is challenging due to the difficulty of isolating excited state coherences in highly congested spectra. In this work, we provide a coherent control scheme that suppresses ground state coherences, thus making rephasing spectra dominated by excited state coherences. We provide a benchmark for the scheme using a model dimeric system and numerically exact methods to analyze the spectral response. We argue that combining temporal and spectral control methods can facilitate a second generation of experiments that are tailored to extract desired information and thus significantly advance our understanding of complex open many-body structure and dynamics.

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• Exact Simulation of Pigment-Protein Complexes Unveils Vibronic Renormalization of Electronic Parameters in Ultrafast Spectroscopy
• Fingerprint and universal Markovian closure of structured bosonic environments
• Systematic coarse-graining of environments for the non-perturbative simulation of open quantum systems
• Two-dimensional spectroscopy beyond the perturbative limit: the influence of finite pulses and detection modes
• Full Microscopic Simulations Uncover Persistent Quantum Effects in Primary Photosynthesis
• Toward Witnessing Molecular Exciton Entanglement from Spectroscopy