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How atoms and electrons in a molecule move during a chemical reaction and how rapidly energy is transferred to or from the surroundings can be studied with flashes of laser light. However, despite prolonged efforts to develop various…
We present a variation of two-dimensional electronic spectroscopy that is capable of mapping spatially-varying differences in electronic couplings using a correlated map of excitation and detection frequencies, with sensitivity orders of…
In recent years, action-detected ultrafast spectroscopies have gained popularity. These approaches offer some advantages over their coherently-detected counterparts, enabling spatially-resolved and operando measurements with high…
Multidimensional optical spectroscopy observes transient excitation dynamics through the time evolution of spectral correlations. Its action-detected variants offer several advantages over the coherent detection and are thus becoming…
Vibrational coherences in ultrafast pump-probe (PP) and 2D electronic spectroscopy (2DES) provide insight into the excited state dynamics of molecules. Femtosecond coherence spectra (FCS) and 2D beat maps yield information about…
Action-detected two-dimensional electronic spectroscopy (A-2DES) could potentially be a versatile chemical tool with applicability across a range of photophysical observables such as photocurrent, photoionization, or fluorescence. However,…
Time-resolved coincidence imaging of photoelectrons and photoions represents the most complete experimental measurement of ultrafast excited state dynamics, a multi-dimensional measurement for a multi-dimensional problem. Here we present…
We present a rapid-scanning approach to fluorescence-detected two-dimensional electronic spectroscopy that combines acousto-optic phase-modulation with digital lock-in detection. The approach shifts the signal detection window to suppress…
Electronic energy transfer in photosynthesis occurs over a range of time scales and under a variety of intermolecular coupling conditions. Recent work has shown that electronic coupling between chromophores can lead to coherent oscillations…
Action-detected two-dimensional electronic spectroscopy (A-2DES) provides valuable insights into ultrafast dynamics within functional materials and devices by measuring incoherent signals like photocurrent. This work details the…
By applying a phase-modulation fluorescence approach to 2D electronic spectroscopy, we studied the conformation-dependent exciton-coupling of a porphyrin dimer embedded in a phospholipid bilayer membrane. Our measurements specify the…
The Fano lineshape arises from the interference of two excitation pathways to reach a continuum. Its generality has resulted in a tremendous success in explaining the lineshapes of many one-dimensional spectroscopies - absorption, emission,…
Two-dimensional electronic spectroscopy (2DES) is one of the most powerful spectroscopic techniques, capable of attaining a nearly complete picture of a quantum system including its couplings, quantum coherence properties and its real-time…
The interaction of exciton and charge transfer (CT) states plays a central role in photo-induced CT processes in chemistry, biology and physics. In this work, we use a combination of two-dimensional electronic spectroscopy (2D-ES),…
Ultrafast laser excitation can trigger multiplex coherent dynamics in molecules. Here, we report attosecond transient absorption experiments addressing simultaneous probing of electronic and vibrational dynamics in a prototype molecule,…
We have previously demonstrated that in the context of two-dimensional (2D) coherent electronic spectroscopy measured by phase modulation and phase-sensitive detection, an \emph{incoherent} nonlinear response, due to pairs of…
We investigate the spectral features of Action-2D Electronic Spectroscopy (A-2DES) in a molecular dimer model across different regimes of excitonic coupling. By explicitly including a second-excited state for each chromophore, we simulate…
Transition metal dichalcogenide, especially MoS2 has attracted lot of attention recently owing to its tunable visible range band gap and anisotropic electronic and transport properties. Here, we report a comprehensive inelastic light…
Moire superlattices in twisted transition metal dichalcogenide bilayers have emerged as a rich platform for exploring strong correlations using optical spectroscopy. Despite observation of rich Mott-Wigner physics stemming from an interplay…
Background-free fluorescence detection in multidimensional electronic spectroscopy promises high sensitivity compared to conventional approaches. Here we explore the sensitivity limits of multidimensional electronic spectroscopy. We present…