Journal ArticleDOI
Tunable two-dimensional femtosecond spectroscopy
TLDR
A two-dimensional Fourier-transform femtosecond spectroscopy technique for the visible spectral region that achieves long-term phase stability by employing diffractive optics and interferometric accuracy of excitation-pulse time delays by using movable glass wedges.Abstract:
We have developed a two-dimensional (2D) Fourier-transform femtosecond spectroscopy technique for the visible spectral region. Three-pulse photon echo signals are generated in a phase-matched noncollinear four-wave mixing box geometry that employs a 3-kHz repetition-rate laser system and optical parametric amplification. Nonlinear signals are fully characterized in amplitude and phase by spectral interferometry. Unlike for previous setups, we achieve long-term phase stability by employing diffractive optics and interferometric accuracy of excitation-pulse time delays by using movable glass wedges. As an example of this technique, 2D correlation and relaxation spectra at 600 nm are shown for a solution of Nile Blue dye in acetonitrile.read more
Citations
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Journal ArticleDOI
Evidence for wavelike energy transfer through quantum coherence in photosynthetic systems
Gregory S. Engel,Gregory S. Engel,Tessa R. Calhoun,Tessa R. Calhoun,Elizabeth L. Read,Elizabeth L. Read,Tae Kyu Ahn,Tae Kyu Ahn,Tomáš Mančal,Tomáš Mančal,Tomáš Mančal,Yuan-Chung Cheng,Yuan-Chung Cheng,Robert E. Blankenship,Graham R. Fleming,Graham R. Fleming +15 more
TL;DR: Previous two-dimensional electronic spectroscopy investigations of the FMO bacteriochlorophyll complex are extended, and direct evidence is obtained for remarkably long-lived electronic quantum coherence playing an important part in energy transfer processes within this system is obtained.
Journal ArticleDOI
Two-dimensional spectroscopy of electronic couplings in photosynthesis
Tobias Brixner,Tobias Brixner,Jens Stenger,Jens Stenger,Harsha M. Vaswani,Harsha M. Vaswani,Minhaeng Cho,Robert E. Blankenship,Graham R. Fleming +8 more
TL;DR: This work directly measures electronic couplings in a molecular complex, the Fenna–Matthews–Olson photosynthetic light-harvesting protein, and finds distinct energy transport pathways that depend sensitively on the detailed spatial properties of the delocalized excited-state wavefunctions of the whole pigment–protein complex.
Journal ArticleDOI
Coherent Two-Dimensional Optical Spectroscopy
TL;DR: Although the optical analogs of 2D NMR do not provide an atomic resolution structure of complex molecules, optical domain multi-dimensional spectroscopy has certain advantages because of the dramatic gain in time resolution possible and the ability to directly observe and quantify the couplings between quantum states involved in molecular dynamical processes.
Journal ArticleDOI
Quantum coherence in photosynthesis for efficient solar-energy conversion
Elisabet Romero,Ramunas Augulis,Vladimir I. Novoderezhkin,Marco Ferretti,Jos Thieme,Jos Thieme,Donatas Zigmantas,Rienk van Grondelle +7 more
TL;DR: The role of coherence in determining the efficiency of charge separation in the plant photosystem II reaction centre is elucidated by comprehensively combining experiment (two-dimensional electronic spectroscopy) and theory (Redfield theory) and it is proposed that this coherent mechanism will inspire the development of new energy technologies.
Journal ArticleDOI
Phase-stabilized two-dimensional electronic spectroscopy
TL;DR: The origin of phase stability and the precise calibration of excitation-pulse time delays using movable glass wedges are discussed and it is shown that correlations between different electronically excited states can be determined from the spectra.
References
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Book
Principles of Nonlinear Optical Spectroscopy
TL;DR: In this article, the authors present a simulation of the optical response functions of a multilevel system with relaxation in a multimode Brownian Oscillator Model and a wavepacket analysis of nonimpulsive measurements.
Journal ArticleDOI
Measuring ultrashort laser pulses in the time-frequency domain using frequency-resolved optical gating
Rick Trebino,Kenneth W. DeLong,David N. Fittinghoff,John N. Sweetser,Marco A. Krumbügel,Bruce A. Richman,Daniel J. Kane +6 more
TL;DR: In this article, the authors summarize the problem of measuring an ultrashort laser pulse and describe in detail a technique that completely characterizes a pulse in time: frequency-resolved optical gating.
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Two-dimensional femtosecond spectroscopy
TL;DR: This review provides an introduction to two-dimensional Fourier transform experiments exploiting second- and third-order vibrational and electronic nonlinearities.
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Linear techniques of phase measurement by femtosecond spectral interferometry for applications in spectroscopy
TL;DR: In this article, dual-quadrature spectral interferometry and Fourier transform (FT) were used to obtain a complete measurement of the complex electric field, E(ω), as a continuous function of frequency.
Journal ArticleDOI
Multidimensional femtosecond correlation spectroscopies of electronic and vibrational excitations.
TL;DR: A classical-oscillator description of these spectroscopies in terms of interacting quasiparticles (rather than transitions among global eigenstates) sets the stage for designing new pulse sequences and inverting the multidimensional signals to yield molecular structures.