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arXiv:1408.2174 · The Journal of Chemical Physics

Multidimensional spectroscopy with a single broadband phase-shaped laser pulse

Rachel Glenn, Shaul Mukamel

Published Apr 9, 2014• 6 citations
arXivHTMLPDF

Abstract

We calculate the frequency-dispersed nonlinear transmission signal of a phase-shaped visible pulse to fourth order in the field. Two phase profiles, a phase-step and phase-pulse, are considered. Two dimensional signals obtained by varying the detected frequency and phase parameters are presented for a three electronic band model system. We demonstrate how two-photon and stimulated Raman resonances can be manipulated by the phase profile and sign, and selected quantum pathways can be suppressed.

DOI
10.1063/1.4869750

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We calculate the frequency-dispersed nonlinear transmission signal of a phase-shaped visible pulse to fourth order in the field. Two phase profiles, a phase-step and phase-pulse, are considered. Two dimensional signals obtained by varying the detected frequency and phase parameters are presented for a three electronic band model system. We demonstrate how two-photon and stimulated Raman resonances can be manipulated by the phase profile and sign, and selected quantum pathways can be suppressed.
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The last two decades have marked a revolution in materials science with the appearance of two novel groups of materials with promising features for future optoelectronics. The first are artificially fabricated metamaterials, composed of carefully engineered nanoparticle arrays, displaying tailored mie and plasmonic resonant responses [1]. The second are atomically thin two-dimensional (2D) semiconductor crystals, characterized by tightly bound excitons, promising for their flexible heterostructure stacking capabilities [2]. In this work we introduce a novel pulse-shaping approach, to study and control the coherent dynamics of resonant quasparticle excitations in such materials. By constructing a state-of-the-art pulse shaper for controlling the spectral phase of our sub-10 fs laser, we tailor the temporal order of instantaneous frequencies driving the noninstantaneous electronic response of the material on resonance [3]. We measure the response to various pulse shapes through monitoring the four-wave mixing (FWM) generation. Our contribution can be described by to three key aspects: We retrace the resonant dispersion by synchronizing the phase-dependent intra-pulse nonlinear wave-mixing with the prediction of the anharmonic oscillator model (AHO). We disentangle the multitude of interfering quantum pathways caused by the resonant dynamics, and reassemble them to achieve a strong nonlinear enhancement as well as near-complete destruction of the nonlinear yield. By controlling two successive resonant states, we present a glimpse into inter-state selectivity. We display nonlinear generation by improving the coherence in one state while suppressing the coherence in another. We believe this work places the control of coherent quasiparticle dynamics in condensed matter systems as a highly appealing field for both fundamental and applied research, such as improved nonlinear sensing, broadband compressed light sources and various ultrafast optoelectronic applications.
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We study theoretically ultrafast modulation spectroscopy in Doppler-broadened cascading three-level and four-level systems. The pump beams consist of two frequency components that drive two-pathway excitation. The four-wave mixing (FWM) signal exhibits damping oscillation as the relative time delay τ between the two pump beams is varied, from which the resonant frequencies between energy levels can be deduced. Furthermore, Doppler-free precision in the measurement of the resonant frequencies can be achieved when the pump beams have either narrow-band or broadband linewidths. We study two-photon resonant FWM induced by time-delayed correlated fluctuating fields in a Doppler-broadened cascading three-level system. It is related intrinsically to the sum-frequency trilevel echo when the pump beams have broadband linewidths. However, unlike the corresponding incoherent-light stimulated photon echo, the maximum of the FWM signal is shifted from τ≃0. If we consider the fluctuations of the pump beams, the FWM signal exhibits damping oscillation when the laser frequency is off resonant from the two-photon transition.
We introduce molecular coherent three-quantum (3Q) two-dimensional (2D) fluorescence spectroscopy with phase cycling via shot-to-shot pulse shaping at a 1 kHz repetition rate. This allows us to acquire simultaneously, within a single scan, three fourth-order and six sixth-order signals correlating various one-quantum, two-quantum, and 3Q coherences. We demonstrate the approach on the dye molecule rhodamine 700 and reproduce all nine 2D data sets, including their absolute signal strengths, with simulations using a single, consistent set of model parameters. We observe a linear concentration dependence of all nonlinear signals, evidencing the absence of cascades and many-particle signals of noninteracting molecules. The single-beam, background-free implementation allows direct comparability between various nonlinear signal types and provides information about multiple excited states. Apart from molecules, the method is expected to be applicable to supramolecular systems, polymers, and solid-state materials with the prospect of revealing signatures of bi- and triexcitonic states.