Selective Enhancements in 2D Fourier Transform Optical Spectroscopy with Tailored Pulse Shapes

Wen, Patrick Y.; Nelson, Keith A.

doi:10.1021/jp401150d

Cited by 13 publications

(10 citation statements)

References 29 publications

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“…Overlapping pathways on a one-quantum spectrum may be separated by spectral filtering of the excitation pulses [38][39][40]. Another method is to acquire zero-quantum spectra, which spectrally separate intraband coherence pathway responses from population state responses directly [32].…”

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confidence: 99%

Non-Markovian Exciton-Phonon Interactions in Core-Shell Colloidal Quantum Dots at Femtosecond Timescales

et al. 2019

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We perform two-dimensional coherent spectroscopy on CdSe/CdZnS core/shell colloidal quantum dots at cryogenic temperatures. In the two-dimensional spectra, sidebands due to electronic coupling with CdSe lattice LO-phonon modes are observed to have evolutions deviating from the exponential dephasing expected from Markovian spectral diffusion, which is instantaneous and memory-less.Comparison to simulations provides evidence that LO-phonon coupling induces energy-gap fluctuations on the finite timescales of nuclear motion. The femtosecond resolution of our technique probes exciton dynamics directly on the timescales of phonon coupling in nanocrystals.

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confidence: 99%

Non-Markovian Exciton-Phonon Interactions in Core-Shell Colloidal Quantum Dots at Femtosecond Timescales

et al. 2019

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“…Shaping the amplitude and phase of femtosecond laser pulses has been used, for example, to control the shape of wavefunctions in atomic systems (11) or to control and optimize the single-photon and multiphoton fluorescence in atoms such as cesium (12) and complex systems, e.g., dye molecules (13). Shaped pulses are also used in time-resolved coherent anti-Stokes Raman scattering (14)(15)(16) or 2D spectroscopy (17,18). Adaptive shaping of the pulses via feedback control even allows the optimization of dynamical processes, e.g., the relative photodissociation yield of organometallic molecules (19), the relative twophoton fluorescence yield of dye molecules (20), and the energy transfer in light-harvesting molecules (21).…”

mentioning

confidence: 99%

Signatures and control of strong-field dynamics in a complex system

Meyer

Liu

Müller

et al. 2015

Proc. Natl. Acad. Sci. U.S.A.

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Controlling chemical reactions by light, i.e., the selective making and breaking of chemical bonds in a desired way with strong-field lasers, is a long-held dream in science. An essential step toward achieving this goal is to understand the interactions of atomic and molecular systems with intense laser light. The main focus of experiments that were performed thus far was on quantum-state population changes. Phase-shaped laser pulses were used to control the population of final states, also, by making use of quantum interference of different pathways. However, the quantum-mechanical phase of these final states, governing the system's response and thus the subsequent temporal evolution and dynamics of the system, was not systematically analyzed. Here, we demonstrate a generalized phase-control concept for complex systems in the liquid phase. In this scheme, the intensity of a control laser pulse acts as a control knob to manipulate the quantum-mechanical phase evolution of excited states. This control manifests itself in the phase of the molecule's dipole response accessible via its absorption spectrum. As reported here, the shape of a broad molecular absorption band is significantly modified for laser pulse intensities ranging from the weak perturbative to the strongfield regime. This generalized phase-control concept provides a powerful tool to interpret and understand the strong-field dynamics and control of large molecules in external pulsed laser fields. C an we find universal concepts to understand and control the response of atoms and molecules in interactions with strong laser fields? This question is at the heart of a vast number of experiments in time-resolved spectroscopy (1-30). The wide range of light sources spanning the spectral range from the X-ray (e.g., free-electron laser sources, synchrotrons) over the visible (conventional laser systems) to the far-infrared regime and covering the temporal range from nanosecond down to attosecond time scales created a wealth of new physics insight into quantum mechanisms, however mostly of simple systems in the gas phase (1-4). In chemistry, the generation of femtosecond laser pulses enabled the investigation of wave packet dynamics in molecules, as the induced vibrations occur on these time scales. Experiments focusing on, for instance, dissociation reactions, atom transfer, isomerization, or solvation dynamics have led to a deeper understanding of chemical bonds and their breakage dynamics and have opened and established the field of femtochemistry (5, 6). The aim is not only to study the light−matter interaction, but to use the obtained understanding of the processes to control the dynamics in complex molecules and, in the future, even to be able to control chemical reactions (7-10). Shaping the amplitude and phase of femtosecond laser pulses has been used, for example, to control the shape of wavefunctions in atomic systems (11) or to control and optimize the single-photon and multiphoton fluorescence in atoms such as cesium (12) and complex systems, e.g....

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“…41 Indeed, any change in the phase of the three pulses will be transferred to the absolute phase of the signal by the aforesaid relation φ 0, s = −φ 0,α + φ 0, β + φ 0,γ . This paves the way to detection schemes where a spectral contribution to the signal can be suppressed or enhanced in a very similar way as in case of background suppression by phase cycling.…”

Section: Phase Shapingmentioning

confidence: 99%

Pulse-shaping assisted multidimensional coherent electronic spectroscopy

Rodríguez

Frei

Cannizzo

et al. 2015

The Journal of Chemical Physics

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Understanding nuclear and electronic dynamics of molecular systems has advanced considerably by probing their nonlinear responses with a suitable sequence of pulses. Moreover, the ability to control crucial parameters of the excitation pulses, such as duration, sequence, frequency, polarization, slowly varying envelope, or carrier phase, has led to a variety of advanced time-resolved spectroscopic methodologies. Recently, two-dimensional electronic spectroscopy with ultrashort pulses has become a more and more popular tool since it allows to obtain information on energy and coherence transfer phenomena, line broadening mechanisms, or the presence of quantum coherences in molecular complexes. Here, we present a high fidelity two-dimensional electronic spectroscopy setup designed for molecular systems in solution. It incorporates the versatility of pulse-shaping methods to achieve full control on the amplitude and phase of the individual exciting and probing pulses. Selective and precise amplitude- and phase-modulation is shown and applied to investigate electronic dynamics in several reference molecular systems.

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Selective Enhancements in 2D Fourier Transform Optical Spectroscopy with Tailored Pulse Shapes

Cited by 13 publications

References 29 publications

Non-Markovian Exciton-Phonon Interactions in Core-Shell Colloidal Quantum Dots at Femtosecond Timescales

Non-Markovian Exciton-Phonon Interactions in Core-Shell Colloidal Quantum Dots at Femtosecond Timescales

Signatures and control of strong-field dynamics in a complex system

Pulse-shaping assisted multidimensional coherent electronic spectroscopy

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