Shaping and spatiotemporal characterization of sub-10-fs pulses focused by a high-NA objective

Pawłowska, Monika; Goetz, Sebastian; Dreher, Christian; Wurdack, Matthias; Krauss, Enno; Razinskas, Gary; Geisler, Peter; Hecht, Bert; Brixner, Tobias

doi:10.1364/oe.22.031496

Cited by 17 publications

(12 citation statements)

References 49 publications

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“…We then utilize the algorithm presented in Ref. 75 Linearly polarized light, acting as a superposition of left-and right-handed circularly polarized light, is used to simultaneously excite both the transitions in the K and K' valleys.…”

Section: Resultsmentioning

confidence: 99%

Exciton–phonon coupling strength in single-layer MoSe2 at room temperature

Trovatello

Conte

et al. 2020

Preprint

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Single-layer transition metal dichalcogenides (1L-TMDs) are at the center of an ever increasing research effort both in terms of fundamental physics and applications. Exciton–phonon coupling (EXPC) plays a key role in determining the photonic and (opto)electronic properties of 1L-TMDs. However, the EXPC strength has not been measured at room temperature. Here, we develop two-dimensional (2D) micro-spectroscopy to determine EXPC of 1L-MoSe2. We detect beating signals as a function of waiting time T, induced by the coupling between the A exciton and the A'1 optical phonon. Analysis of 2D beating maps provides the EXPC with the help of simulations. The Huang–Rhys factor of ~1 is larger than in most other inorganic semiconductor nanostructures. Our technique offers a unique tool to measure EXPC also in other 1L-TMDs and heterogeneous semiconducting systems with a spatial resolution ~260 nm, and will provide design-relevant parameters for the development of novel optoelectronic devices.

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Section: Resultsmentioning

confidence: 99%

Exciton–phonon coupling strength in single-layer MoSe2 at room temperature

Trovatello

Conte

et al. 2020

Preprint

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“… 17 , 18 Application of sophisticated pulse-shaping techniques have recently shown that it is possible to combine ultrashort near-IR pulses (∼800 nm, sub-10 fs), which have become ubiquitous in ultrafast spectroscopy, with high spatial resolution provided by high numerical aperture (NA) objectives. 37 The extension toward the visible spectral region, where many of the most studied materials are strongly active, however, has been lacking.…”

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confidence: 99%

Sub-10 fs Time-Resolved Vibronic Optical Microscopy

Schnedermann

Lim

Wende

et al. 2016

J. Phys. Chem. Lett.

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We introduce femtosecond wide-field transient absorption microscopy combining sub-10 fs pump and probe pulses covering the complete visible (500–650 nm) and near-infrared (650–950 nm) spectrum with diffraction-limited optical resolution. We demonstrate the capabilities of our system by reporting the spatially- and spectrally-resolved transient electronic response of MAPbI3–xClx perovskite films and reveal significant quenching of the transient bleach signal at grain boundaries. The unprecedented temporal resolution enables us to directly observe the formation of band-gap renormalization, completed in 25 fs after photoexcitation. In addition, we acquire hyperspectral Raman maps of TIPS pentacene films with sub-400 nm spatial and sub-15 cm–1 spectral resolution covering the 100–2000 cm–1 window. Our approach opens up the possibility of studying ultrafast dynamics on nanometer length and femtosecond time scales in a variety of two-dimensional and nanoscopic systems.

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“…In case of spatially distorted mode profiles, other techniques that are based on nanoscale probes, not directly relying on the mode profile, can be used (see e.g.Refs. 22,32).At the same time, the graphene four-wave mixing is an extremely efficient process leading to easily detectable signals reaching photon count rates of several millions per second. Most importantly, its spectrally uniform response should allow for phase characterization of laser pulses reaching from the THz to the visible regime.Near-degenerate FWM avoids drawbacks of schemes relying on higher harmonic detection and the associated requirements regarding the achromaticity and the large spectral detection range as discussed in the following.…”

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confidence: 99%

Graphene Near-Degenerate Four-Wave Mixing for Phase Characterization of Broadband Pulses in Ultrafast Microscopy

et al. 2015

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We investigate near-degenerate four-wave mixing in graphene using femtosecond laser pulse shaping microscopy. Intense near-degenerate four-wave mixing signals on either side of the exciting laser spectrum are controlled by amplitude and phase shaping. Quantitative signal modeling for the input pulse parameters shows a spectrally flat phase response of the near-degenerate four-wave mixing due to the linear dispersion of the massless Dirac Fermions in graphene. Exploiting these properties we demonstrate that graphene is uniquely suited for the intrafocus phase characterization and compression of broadband laser pulses, circumventing disadvantages of common methods utilizing second or third harmonic light.

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Shaping and spatiotemporal characterization of sub-10-fs pulses focused by a high-NA objective

Cited by 17 publications

References 49 publications

Exciton–phonon coupling strength in single-layer MoSe2 at room temperature

Exciton–phonon coupling strength in single-layer MoSe2 at room temperature

Sub-10 fs Time-Resolved Vibronic Optical Microscopy

Graphene Near-Degenerate Four-Wave Mixing for Phase Characterization of Broadband Pulses in Ultrafast Microscopy

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