Related papers: Extracting double-quantum coherence in two-dimensi…
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…
Selecting distinct quantum pathways in two-dimensional electronic spectroscopy (2DES) can give particularly deep insights into coherent and incoherent interactions and quantum dynamics in various materials. This includes isolating rephasing…
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…
Recent studies have shown that the nonlinear optical response of crystalline systems is fundamentally a quantum geometric property. In this work, we propose two-dimensional coherent spectroscopy (2DCS), which measures the nonlinear…
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 employ two-dimensional (2D) coherent, nonlinear spectroscopy to investigate couplings within individual InAs quantum dots (QD) and QD molecules. Swapping pulse ordering in a two-beam sequence permits to distinguish between rephasing and…
We present a widefield two-dimensional electronic spectroscopy microscope (2DESM) that integrates multidimensional coherent spectroscopy with optical imaging, enabling femtosecond temporal and micrometer spatial resolution. The broadband…
The origin of the coherences in two-dimensional spectroscopy of photosynthetic complexes remains disputed. Recently it has been shown that in the ultrashort-pulse limit, oscillations in a frequency-integrated pump-probe signal correspond…
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…
Two-dimensional (2D) spectroscopy uses multiple electromagnetic pulses to infer the properties of a complex system. A paradigmatic class of target systems are molecular aggregates, for which one can obtain information on the eigenstates,…
Two-dimensional spectroscopy (2DS) is a powerful ultrafast technique for probing electronic and vibrational dynamics in complex microscopic systems. Extracting detailed information on system dynamics and system-bath interactions from 2DS…
Two-dimensional electronic spectroscopy (2DES) is a powerful tool for exploring quantum effects in energy transport within photosynthetic systems and investigating novel material properties. However, simulating the dynamics of these…
Optical two-dimensional coherent spectroscopy (2DCS) has become a powerful tool for studying energy level structure, dynamics, and coupling in many systems including atomic ensembles. Various types of two-dimensional (2D) spectra, including…
Double-quantum two-dimensional coherent spectroscopy (MDCS) is a powerful optical method that is used to study optical properties of atomic and complex molecular systems and semiconductor materials. Double-quantum 2D spectra and…
The geometric phase is a fundamental quantum mechanical phenomenon uniquely associated with conical intersections (CI) between potential energy surfaces and serves as a definitive signature of their presence. In this study, we propose a…
Is it possible to infer the time evolving quantum state of a multichromophoric system from a sequence of two-dimensional electronic spectra (2D-ES) as a function of waiting time? Here we provide a positive answer for a tractable model…
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…
We report the observation of double-quantum coherence signals in a gas of potassium atoms at twice the frequency of the one-quantum coherences. Since a single atom does not have a state at the corresponding energy, this observation must be…
Femtosecond coherent multidimensional spectroscopy is demonstrated for an ultracold gas. For this, a setup for phase modulation spectroscopy is used to probe the $3^2\mathrm{S}_{1/2} - 2^2\mathrm{P}_{1/2, 3/2}$ transition in an 800…
Two-dimensional spectroscopy is discussed for open quantum systems with multiple simultaneously measurable fluxes. In particular, we discuss a junction where optical measurements of photon flux are complemented with simultaneous transport…