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Simultaneous Characterization of Two Ultrashort Optical Pulses at Different Frequencies Using a WS₂ Monolayer.

Marcus L Noordam¹, Javier Hernandez-Rueda¹, L Kuipers¹

¹Kavli Institute of Nanoscience Delft, Department of Quantum Nanoscience, Delft University of Technology, Lorentzweg 1, 2628 CJ Delft, The Netherlands.

|June 21, 2022

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This study uses a WS₂ monolayer and an adjusted FROG algorithm to simultaneously characterize two ultrashort laser pulses. The method accurately retrieves pulse intensity and phase using combined nonlinear optical signals.

Area of Science:

Nonlinear Optics
Materials Science
Ultrafast Spectroscopy

Background:

Precise characterization of ultrashort laser pulses is crucial for scientific advancement.
Frequency-Resolved Optical Gating (FROG) is a standard technique for pulse retrieval.
Existing methods face challenges in simultaneously characterizing multiple pulses.

Purpose of the Study:

To develop a novel method for simultaneous characterization of two ultrashort laser pulses with different frequencies.
To leverage the nonlinear optical properties of a WS₂ monolayer for enhanced pulse diagnostics.
To introduce an adjusted double-blind FROG algorithm for improved pulse retrieval accuracy.

Main Methods:

Utilized a WS₂ monolayer for its broad-band nonlinear optical response.

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Employed relaxed phase-matching conditions for simultaneous Four-Wave Mixing (FWM) and Sum-Frequency Generation (SFG) spectral acquisition.

Developed and applied an adjusted double-blind FROG algorithm using iterative fast Fourier transforms on combined FWM and SFG FROG traces.

Main Results:

Successfully retrieved the intensity and phase of two simultaneously interacting ultrashort laser pulses.
Demonstrated agreement between computed and observed FROG traces for both FWM and SFG processes.
Validated the retrieved pulse shapes using a Second-Harmonic Generation (SHG) FROG trace and nondegenerate cross-correlation measurements.

Conclusions:

The WS₂ monolayer offers a versatile platform for simultaneous characterization of multiple ultrashort laser pulses.
The adjusted double-blind FROG algorithm effectively extracts pulse information from combined nonlinear optical signals.
Nonlinearly generated photoluminescence (PL) from WS₂ provides complementary autocorrelation and cross-correlation data.