Related papers: Two-Dimensional Electronic Spectroscopy Using Inco…
Recent interest in the role of quantum mechanics in the primary events of photosynthetic energy transfer has led to a convergence of nonlinear optical spectroscopy and quantum optics on the topic of energy-transfer dynamics in…
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…
We perform a beat-frequency-resolved analysis for two-dimensional electronic spectroscopy using a high-speed and stable 2D electronic spectrometer and few-cycle visible laser pulses to disentangle the vibrational coherences in an artificial…
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…
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…
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…
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…
Multidimensional coherent optical spectroscopy is one of the most powerful tools for investigating complex quantum mechanical systems. While it was conceived decades ago in magnetic resonance spectroscopy using micro- and radio-waves, it…
We report a conceptually straightforward witness that isolates coherent electronic oscillations from their vibronic counterparts in nonlinear optical spectra of molecular aggregates: Coherent oscillations as a function of waiting time in…
This is the first in a series of two papers investigating the effect of electron-phonon coupling in two-dimensional Fourier transformed electronic spectroscopy. We present a series of one- and two-dimensional nonlinear spectroscopic…
We analyze electronically excited nuclear wave functions and their coherence when subjecting a molecule to the action of natural, pulsed incoherent solar-like light, and to that of ultrashort coherent light assumed to have the same center…
The correlated behavior of electrons determines the structure and optical properties of molecules, semiconductor and other systems. Valuable information on these correlations is provided by measuring the response to femtosecond laser…
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 theoretical and experimental results showing the effects of incoherent population mixing on two-dimensional (2D) coherent excitation spectra that are measured via a time-integrated population and phase-sensitive detection. The…
Two-dimensional electronic spectra (2DES) provide unique ways to track the energy transfer dynamics in light-harvesting complexes. The interpretation of the peaks and structures found in experimentally recorded 2DES is often not…
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 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…
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…
Giant strides in ultrashort laser pulse technology have enabled real-time observation of dynamical processes in complex molecular systems. Specifically, the discovery of oscillatory transients in the two-dimensional electronic spectra of…
The light-harvesting efficiency of a photoactive molecular complex is largely determined by the properties of its electronic quantum states. Those, in turn, are influenced by molecular vibrational states of the nuclear degrees of freedom.…