Pulse Propagation Effects in Optical 2D Fourier-Transform Spectroscopy: Experiment

Li, Hebin; Spencer, Austin P.; Kortyna, Andrew; Jonas, David M.; Cundiff, Steven T.

doi:10.1021/jp4007872

Cited by 27 publications

(55 citation statements)

References 47 publications

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“…For both CsPbBr 3 and MAPbBr 3 in the orthorhombic phase, the exceptionally large spread in Kerr effect frequency and the abrupt decay at t 1 are unphysical for coherent phonons or other collective modes. As suggested in early FWM studies, light propagation can strongly affect FWM signals and especially 2D spectroscopy line shapes in isotropic media such as dense gases (36,37), solutions (38), or cubic semiconductors (39). In LHPs, anisotropic light propagation seems to play a crucial role.…”

Section: Resultsmentioning

confidence: 91%

Decoding ultrafast polarization responses in lead halide perovskites by the two-dimensional optical Kerr effect

Maehrlein

Joshi

Huber

et al. 2021

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

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The ultrafast polarization response to incident light and ensuing exciton/carrier generation are essential to outstanding optoelectronic properties of lead halide perovskites (LHPs). A large number of mechanistic studies in the LHP field to date have focused on contributions to polarizability from organic cations and the highly polarizable inorganic lattice. For a comprehensive understanding of the ultrafast polarization response, we must additionally account for the nearly instantaneous hyperpolarizability response to the propagating light field itself. While light propagation is pivotal to optoelectronics and photonics, little is known about this in LHPs in the vicinity of the bandgap where stimulated emission, polariton condensation, superfluorescence, and photon recycling may take place. Here we develop two-dimensional optical Kerr effect (2D-OKE) spectroscopy to energetically dissect broadband light propagation and dispersive nonlinear polarization responses in LHPs. In contrast to earlier interpretations, the below-bandgap OKE responses in both hybrid CH3NH3PbBr3 and all-inorganic CsPbBr3 perovskites are found to originate from strong hyperpolarizability and highly anisotropic dispersions. In both materials, the nonlinear mixing of anisotropically propagating light fields results in convoluted oscillatory polarization dynamics. Based on a four-wave mixing model, we quantitatively derive dispersion anisotropies, reproduce 2D-OKE frequency correlations, and establish polarization-dressed light propagation in single-crystal LHPs. Moreover, our findings highlight the importance of distinguishing the often-neglected anisotropic light propagation from underlying coherent quasiparticle responses in various forms of ultrafast spectroscopy.

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Section: Resultsmentioning

confidence: 91%

Decoding ultrafast polarization responses in lead halide perovskites by the two-dimensional optical Kerr effect

Maehrlein

Joshi

Huber

et al. 2021

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

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“…(2). We note that the sample here is considered optically thin, in which case the spectral distortion due to pulse propagation effects [35,36] is negligible.…”

Section: Implementation Of 3d Coherent Spectroscopymentioning

confidence: 99%

Interpretation of optical three-dimensional coherent spectroscopy

Titze

2017

Phys. Rev. A

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As an extension to powerful Two-Dimensional Coherent Spectroscopy (2DCS), optical Three-Dimensional Coherent Spectroscopy (3DCS) has been experimentally implemented and found beneficial in studying various systems in physics and chemistry. A critical challenge is how to interpret 3D spectra and extract useful quantitative information, given the richness and complexity of 3D data. Here, we demonstrate how the information of a system's optical response is manifested in 3D spectra by theoretical simulations of a few representative examples including a homogeneous three-level V system, an inhomogeneous three-level V system, and an inhomogeneous three-level ladder system. These examples show that important parameters of the system can be extracted from the spectral pattern, peak positions, amplitudes, and line shapes. The method developed here can be used to analyze 3D spectra of more sophisticated systems which might be a generalization or combination of the three examples, contributing to develop a general approach for the interpretation of 3D spectra.

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“…The signal is spectrally resolved by a grating-based spectrometer on a CCD camera -providing, in a single acquisition, the Fourier transform of the signal with respect to emission time t. Phase resolution is obtained through spectral interferometry [36], where the signal is heterodyned with a reference pulse (local oscillator (LO)). The LO can either be routed around the sample [33,34] or through the sample [31,35], in which case the amplitude and phase distortion of the LO needs to be accounted and compensated for [37]. Based on a similar principle, the use of the box geometry in a reflection geometry has also been demonstrated [38], and can be used in the case of optically dense samples.…”

Section: Box Geometrymentioning

confidence: 99%

Multidimensional coherent optical spectroscopy of semiconductor nanostructures: a review

Nardin

2015

Semicond. Sci. Technol.

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Abstract. Multidimensional Coherent optical Spectroscopy (MDCS) is an elegant and versatile tool to measure the ultrafast nonlinear optical response of materials. Of particular interest for semiconductor nanostructures, MDCS enables the separation of homogeneous and inhomogeneous linewidths, reveals the nature of coupling between resonances, and is able to identify the signatures of many-body interactions. As an extension of transient Four-Wave Mixing (FWM) experiments, MDCS can be implemented in various geometries, in which different strategies can be used to isolate the FWM signal and measure its phase. I review and compare different practical implementations of MDCS experiments adapted to the study of semiconductor materials. The power of MDCS is illustrated by discussing experimental results obtained on semiconductor nanostructures such as quantum dots, quantum wells, microcavities, and layered semiconductors.

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Pulse Propagation Effects in Optical 2D Fourier-Transform Spectroscopy: Experiment

Cited by 27 publications

References 47 publications

Decoding ultrafast polarization responses in lead halide perovskites by the two-dimensional optical Kerr effect

Decoding ultrafast polarization responses in lead halide perovskites by the two-dimensional optical Kerr effect

Interpretation of optical three-dimensional coherent spectroscopy

Multidimensional coherent optical spectroscopy of semiconductor nanostructures: a review

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