Crossing disciplines ‐ A view on two‐dimensional optical spectroscopy

Abstract

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, condensed matter and quantum physics on the topic of energy-transfer dynamics in pigment-protein complexes. The convergence of these communities has unveiled a mismatch between the background and terminology of the respective fields. To make connections, a pedagogical guide to understanding the basics of two-dimensional spectra is provided, aimed at researchers with a background in quantum mechanics and condensed matter.

Optimizing sparse sampling for 2D electronic spectroscopy

“…Coherent two-dimensional (2D) electronic spectroscopy [1][2][3][4][5] has become an established method to study, among others, energy transfer in light harvesting complexes, [6][7][8] electronic dynamics in semiconductors, [9][10][11][12][13] plasmonic coherences, 14 and photochemical reactions. 15 Most of the experimental realizations rely on the non-collinear box geometry and heterodyned detection of a coherent optical signal.…”

Probing polaron excitation spectra in organic semiconductors by photoinduced-absorption-detected two-dimensional coherent spectroscopy

“…Multidimensional electronic spectroscopy (ES) developed in analogy to the counterpart of nuclear magnetic resonance has become a powerful tool to study the electronic dynamics of macromolecular systems [1][2][3]. By probing nonlinear optical responses and spreading them along two time/frequency axes, such spectroscopic experiments reveal transient correlations between specific electronic transitions with femtosecond temporal resolution [4,5].…”

Ultra-broadband 2D electronic spectroscopy of carotenoid-bacteriochlorophyll interactions in the LH1 complex of a purple bacterium

“…The dynamics of electronic excitations in both LH2 and LH1 complexes have been extensively studied by a variety of ultrafast spectroscopy approaches, including pump-probe and fluorescence upconversion. 23 The advent of two-dimensional electronic spectroscopy (2DES) has for the first time enabled the combination of the highest temporal and spectral resolution, [24][25][26][27] thanks to the Fourier transform analysis in the frequency domain. In a 2DES experiment, the system under study is excited by three consecutive pulses, with controllable relative delays t 1 (coherence time) and t 2 (population or waiting time).…”