相关论文: Disentangling Single- and Biexciton Dynamics with …
Two-dimensional (2D) fluorescence-excitation (2D-FLEX) spectroscopy is a recently proposed nonlinear femtosecond technique for the detection of photoinduced dynamics. The method records a time-resolved fluorescence signal in its excitation-…
We present calculations of the fluorescence-detected coherent two-dimensional (F-2DES) spectra of a molecular heterodimer. We compare how the F-2DES technique differs from the standard coherently detected two-dimensional (2DES) spectroscopy…
In molecular aggregates, multiple delocalized exciton states interact with phonons, making the state-resolved spectroscopic monitoring of dynamics challenging. We propose a protocol that combines photon-entanglement-enhanced narrowband…
Two-dimensional (2D) spectroscopy provides information about dissipative processes subsequent to electronic excitation, which play a functional role in energy harvesting materials and devices. This technique is particularly sensitive to…
Two-dimensional electronic spectroscopy provides information on coupling and energy transfer between excited states on ultrafast timescales. Only recently, incoherent fluorescence detection has made it possible to combine this method with…
The prevalence of long-lasting oscillatory signals in the 2d echo-spectroscopy of light-harvesting complexes has led to a search for possible mechanisms. We investigate how two causes of oscillatory signals are intertwined: (i) electronic…
Excitons -- bound electron-hole pairs -- play a central role in light-matter interaction phenomena, and are crucial for wide-ranging applications from light harvesting and generation to quantum information processing. A long-standing…
The response of matter to an optical excitation consists essentially of absorption and emission. Traditional spectroscopy accesses the frequency-resolved and time-integrated response, while the temporal evolution stays concealed. However,…
Nonlinear spectroscopic techniques using entangled photon pairs can provide an opportunity to exploit non-classical correlations encoded in two-photon wavefunctions to manipulate two-exciton wavefunctions. We propose an entangled photon…
We present the extension of the time-dependent configuration interaction singles (TDCIS) method to the computation of the electron kinetic-energy spectrum in photoionization processes. Especially for strong and long ionizing light pulses…
Pulsed electrostatic gating combined with capacitive charge sensing is used to perform excited state spectroscopy of an electrically isolated double-quantum-dot system. The tunneling rate of a single charge moving between the two dots is…
Techniques for coherent multidimensional optical spectroscopy have been developed and utilised to understand many different processes, including energy transfer in photosynthesis and many-body effects in semiconductor nanostructures.…
We introduce two-quantum (2Q) fluorescence-detected pump-probe (F-PP) spectroscopy as a tool to probe ultrafast multiparticle interactions in many-body systems. We describe a pulse-shaper-based fully collinear setup utilizing phase cycling…
Non-equilibrium photon correlations of coherently excited single quantum systems can reveal their internal quantum dynamics and provide spectroscopic access. Here we propose and discuss the fundamentals of a coherent photon coincidence…
The electronic and nuclear dynamics in methanol, following 156~nm photoexcitation, are investigated by combining a detailed analysis of time-resolved photoelectron spectroscopy experiments with electronic structure calculations. The…
Single-molecule fluorescence spectroscopy is a powerful method that avoids ensemble averaging, but its temporal resolution is limited by the fluorescence lifetime to nanoseconds at most. At the ensemble level, two-dimensional spectroscopy…
Molecular absorption and photo-electron spectra can be efficiently predicted with real-time time-dependent density-functional theory (TDDFT). We show here how these techniques can be easily extended to study time-resolved pump-probe…
Recent theoretical studies in quantum spectroscopy have emphasized the potential of non-classical correlations in entangled photon pairs for selectively targeting specific nonlinear optical processes in nonlinear optical responses. However,…
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…
Ultra-fast and multi-dimensional spectroscopy gives a powerful looking glass into the dynamics of molecular systems. In particular two-dimensional electronic spectroscopy (2DES) provides a probe of coherence and the flow of energy within…