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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…

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…

Fluorescence-detected two-dimensional electronic spectroscopy (F-2DES) projects the third-order non-linear polarization in a system as an excited electronic state population which is incoherently detected as fluorescence. Multiple variants…

Two-dimensional electronic spectroscopy (2DES) provides rich information about how the electronic states of molecules, proteins, and solid-state materials interact with each other and their surrounding environment. Atomistic molecular…

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…

量子物理 · 物理学 2021-03-31 André Anda , Jared H. Cole

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…

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 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,…

化学物理 · 物理学 2017-09-06 Daniel Finkelstein-Shapiro , Felipe Poulsen , Tõnu Pullerits , Thorsten Hansen

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…

化学物理 · 物理学 2024-06-07 Dale Green , Giovanni Bressan , Ismael A. Heisler , Stephen R. Meech , Garth A. Jones

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,…

The coupling between electronic excitations and collective bosonic modes is fundamental to the emergence of high-temperature superconductivity in cuprates. Despite extensive effort, conventional equilibrium and pump-probe optical…

Ultrafast electron microscopy (UEM) has found widespread applications in physics, chemistry, and materials science, enabling real-space imaging of dynamics on ultrafast timescales. Recent advances have pushed the temporal resolution of UEM…

Imaging the structure of molecules in transient excited states remains a challenge due to the extreme requirements for spatial and temporal resolution. Ultrafast electron diffraction from aligned molecules (UEDAM) provides atomic resolution…

原子物理 · 物理学 2015-10-23 Jie Yang , Joshua Beck , Cornelis J. Uiterwaal , Martin Centurion

Defects in solid-state materials play a central role in determining coherence, stability, and performance in quantum technologies. Although narrowband techniques can probe specific resonances with high precision, a broadband spectroscopic…

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…

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…

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…

原子物理 · 物理学 2023-01-16 Friedemann Landmesser , Tobias Sixt , Katrin Dulitz , Lukas Bruder , Frank Stienkemeier

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…

The development of attosecond technology has enabled the real-time observation of coherent electron motion in atoms, molecules and condensed phases. Experimentally, it is now possible to generate laser pulses of durations of only a few tens…

化学物理 · 物理学 2017-05-18 David Ayuso

Laser dynamics underpin a broad range of modern photonic technologies and continue to reveal rich nonlinear behaviors. However, existing spectroscopic tools, most notably time-stretched dispersive Fourier transform spectroscopy (TS-DFT),…

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