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Numerical method for nonlinear optical spectroscopies: Ultrafast ultrafast spectroscopy.

Peter A Rose¹, Jacob J Krich¹

¹Department of Physics, University of Ottawa, Ottawa, Ontario K1N 6N5, Canada.

The Journal of Chemical Physics

|June 10, 2019

Summary

We introduce Ultrafast Ultrafast (UF²) spectroscopy, a novel numerical method for calculating n-wave mixing signals. This efficient technique simplifies complex calculations, offering identical results to standard methods with enhanced computational speed.

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Area of Science:

Quantum optics
Computational chemistry
Spectroscopy

Background:

Calculating n-wave mixing signals is crucial for understanding light-matter interactions.
Existing methods for computing nth-order wavepackets can be computationally intensive.
Ultrafast Ultrafast (UF²) spectroscopy offers a new approach to this challenge.

Purpose of the Study:

To introduce and validate a novel numerical method, Ultrafast Ultrafast (UF²) spectroscopy.
To demonstrate the computational efficiency and simplicity of the UF² method.
To provide a user-friendly tool for calculating n-wave mixing signals.

Main Methods:

The UF² method utilizes nonperturbative and costless propagation of system time-evolution.
Numerical propagation is performed only during the nonzero duration of perturbative optical pulses.
The fast Fourier transform convolution algorithm is employed for efficient numerical propagation.

Main Results:

The UF² method achieves significant computational speed-ups compared to existing techniques.
Spectra calculated using UF² are identical to those obtained from the standard response function formalism.
The method is demonstrated to be broadly applicable across various use cases.

Conclusions:

UF² spectroscopy provides a computationally efficient and simple alternative for calculating n-wave mixing signals.
The method's ease of implementation facilitates its adoption in research.
This technique simplifies the complex understanding of n-wave mixing processes, analogous to Feynman diagrams.