Beating spatio-temporal coupling: implications for pulse shaping and coherent control experiments

Brinks, Daan; Hildner, Richard; Stefani, Fernando D.; Hulst, N.F. van

doi:10.1364/oe.19.026486

Cited by 42 publications

(43 citation statements)

References 57 publications

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“…More importantly, the results show that femtosecond pulses can be delivered to nanometric probes unperturbed by, e.g., spatiotemporal coupling 23,24 or by the probe itself. Moreover, nonlinear signals and phase information can be reliably extracted from deep subwavelength volumes, which is an important prerequisite for accurate nonlinear nanoscopy.…”

Section: Control Of Fsmentioning

confidence: 93%

“…In other words, there is no measurable spectral phase inhomogeneity inside the focal volume. 23,24 The ability to test for spatiotemporal inhomogeneities inside the excitation spot is a unique advantage of using NPs as opposed to SH bulk crystals and provides a tool for correctly designing pulse-shaping experiments on the nanoscale.…”

Section: Control Of Fs Pulses For Ultrafast Nanophotonics N Accanto Ementioning

confidence: 99%

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Phase control of femtosecond pulses on the nanoscale using second harmonic nanoparticles

et al. 2014

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Investigations of ultrafast processes occurring on the nanoscale require a combination of femtosecond pulses and nanometer spatial resolution. However, controlling femtosecond pulses with nanometer accuracy is very challenging, as the limitations imposed both by dispersive optics on the time duration of a pulse and by the spatial diffraction limit on the focusing of light must be overcome simultaneously. In this paper, we provide a universal method that allows full femtosecond pulse control in subdiffraction-limited areas. We achieve this aim by exploiting the intrinsic coherence of the second harmonic emission from a single nonlinear nanoparticle of deep subwavelength dimensions. The method is proven to be highly sensitive, easy to use, quick, robust and versatile. This approach allows measurements of minimal phase distortions and the delivery of tunable higher harmonic light in a nanometric volume. Moreover, the method is shown to be compatible with a wide range of particle sizes, shapes and materials, allowing easy optimization for any given sample. This method will facilitate the investigation of light-matter interactions on the femtosecond-nanometer level in various areas of scientific study.

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Section: Control Of Fsmentioning

confidence: 93%

Section: Control Of Fs Pulses For Ultrafast Nanophotonics N Accanto Ementioning

confidence: 99%

Phase control of femtosecond pulses on the nanoscale using second harmonic nanoparticles

et al. 2014

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“…To this end, pulse-shaping techniques were combined with confocal microscopy that allows to efficiently collect the fluorescence signal of single objects. [104,105] The general idea behind this approach is to excite a single molecule with a sequence of two ultrashort pulses with controlled delay time as well as phase difference between the pulses. The first pulse creates coherences between the ground and excited electronic states or coherences between excited states (electronic or vibronic).…”

Section: Observation Of Ultrafast Excited-state Dynamics In Single Momentioning

confidence: 99%

Exciton Transport in Molecular Aggregates – From Natural Antennas to Synthetic Chromophore Systems

Brixner

Hildner

Köhler

et al. 2017

Advanced Energy Materials

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301

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The transport of excitation energy in molecular aggregates is of crucial importance for the function of organic optoelectronic devices and next‐generation solar cells. First, this review summarizes the theoretical background of the nature of the electronically excited states of molecular aggregates. For these systems, the electronic interaction between the monomers leads to the formation of exciton states. This goes along with a shift of the excitation energies and a redistribution of the oscillator strength with respect to the monomers. Next, a brief overview is provided over experimental techniques that allow to study the properties of excitons in molecular aggregates. This includes single‐molecule spectroscopy, coherent two‐dimensional (2D) spectroscopy, and single‐molecule coherent spectroscopy. Finally, examples of molecular aggregates spanning the range from natural systems that act in photosynthesis as light‐harvesting antennas to artificial aggregates built from synthetic chromophores are illustrated.

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“…The former can be minimized by employing a double pass 4f pulse shaper setup. [15] The latter can be explained as follows.…”

Section: Challenges Of Miipsmentioning

confidence: 99%

Compression of ultrashort laser pulses via gated multiphoton intrapulse interference phase scans

Comin¹,

Ciesielski²,

Piredda³

et al. 2014

J. Opt. Soc. Am. B

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Delivering femtosecond laser light in the focal plane of a high numerical aperture microscope objective is still a challenge, despite significant developments in the generation of ultrashort pulses. One of the most popular techniques, used to correct phase distortions resulting from propagation through transparent media, is the multiphoton intrapulse interference phase scan (MIIPS). The accuracy of MIIPS however is limited when higher order phase distortions are present. Here we introduce an improvement, called Gated-MIIPS, which avoids shortcomings of MIIPS, reduces the influence of higher order phase terms, and can be used to more efficiently compress broad band laser pulses even with a simple 4f pulse shaper setup. In this work we present analytical formulas for MIIPS and Gated-MIIPS valid for chirped Gaussian pulses; we show an approximated analytic expression for Gated-MIIPS valid for arbitrary pulse shapes; finally we demonstrate the increased accuracy of Gated-MIIPS via experiment and numerical simulation. This paper was published in Journal of the Optical Society of America B and is made available as an electronic reprint with the permission of OSA. The paper can be found at the following URL on the OSA website: http://www.opticsinfobase.org. Systematic or multiple reproduction or distribution to multiple locations via electronic or other means is prohibited and is subject to penalties under law.

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Beating spatio-temporal coupling: implications for pulse shaping and coherent control experiments

Cited by 42 publications

References 57 publications

Phase control of femtosecond pulses on the nanoscale using second harmonic nanoparticles

Phase control of femtosecond pulses on the nanoscale using second harmonic nanoparticles

Exciton Transport in Molecular Aggregates – From Natural Antennas to Synthetic Chromophore Systems

Compression of ultrashort laser pulses via gated multiphoton intrapulse interference phase scans

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