arXiv subjects

Francis Walz

Publications and source records attributed to Francis Walz.

5 recordsLinked to original sources

arXiv2025

Attosecond Control of Squeezed Light

Squeezed light is a key resource in quantum metrology and quantum information science. It is primarily generated through nonlinear optical interactions, where the degree of squeezing is set by the nonlinearity of the medium. Here, we modulate the third-order nonlinear response of a dielectric with strong ultrafast laser fields to control squeezed light generation on attosecond time scales. By tuning a sub-cycle phase delay between the input femtosecond pulses, we switch the generated light between amplitude-squeezed and phase-squeezed states. We measure the quantum noise using a frequency-resolved balanced homodyne detection scheme that extracts field quadratures in many frequency modes simultaneously. From these measurements we obtain the complete coherency matrix containing quadrature correlations across the frequency modes of the pulse. These results enable quantum light sources with sub-cycle control of squeezing and open a route to transduction of dynamical quantum correlations in matter to quantum correlations in electric fields.

quant-ph↗

arXiv2025

Strong-field Driven Sub-cycle Band Structure Modulation and Dephasing Control

Over the past decade, ultrafast electron dynamics in the solid state have been extensively studied using various strong light-matter interaction techniques, such as high-harmonic generation. These studies lead to multiple interpretations of light-matter interaction in the strong-field regime, with exact mechanisms not yet fully understood. It is well known that strong-field interaction with a crystalline solid leads to significant modification of its band structure and, hence, its optical properties on ultrafast timescales. In this work, we present measurements of ultrafast electric-field observables in magnesium oxide using a non-resonant nonlinear optical interaction. Using field observables, we show that strong laser fields modulate the band structure on sub-cycle timescales, thereby altering the material's nonlinear optical response. We perform time-dependent perturbation theory calculations using a field-dependent dispersion relation and non-perturbative semiconductor Bloch equation calculations, both of which agree with experimental observations. Furthermore, we directly extract dephasing times from the real-time signal electric field envelope and show sub-cycle control of dephasing times. Our work offers a new perspective on strong-field-driven electron dynamics in solids through electric-field observables. The demonstrated attosecond modulation of the nonlinear response could have important implications for quantum light generation and quantum spectroscopy using nonlinear optical processes.

physics.optics↗

arXiv2025

Femtosecond Temporal Phase-Resolved Nonlinear Optical Spectroscopy in Molecules with Lock-in Enabled Phase Tracking

We describe an experiment to measure the emitted real-time electric field from an ultrafast third-order nonlinear optical interaction in molecules, using a phase-tracked spectral interferometry scheme. By combining a software lock-in amplification based spectrometer with spectral interferometry, we measure the electric field of the nonlinear optical signal from rotationally excited gas-phase molecules. The lock-in spectrometer allows selective measurement of signals of interest with improved signal-to-noise ratio, while rejecting any unwanted incoherent background. The nonlinear optical signal interferes with a known reference pulse on the spectrometer, which allows measurement of ultraweak signal electric fields. Further, we show that lock-in detection enables correction of slow interferometric drifts by utilizing a multidimensional measurement space. Thus, interferometric stability is achieved without the need for active stabilization, which typically utilizes an independent phase drift measurement. We present data from an experiment in impulsively aligned molecules that demonstrates the important features of our scheme. The scheme can be applied to study ultrafast dynamics in laser excited systems in the gas, liquid, and solid phases of matter.

physics.optics↗

arXiv2023

Ultrafast Field-Resolved Nonlinear Optical Spectroscopy in the Molecular Frame

We resolve the real-time electric field of a femtosecond third-order nonlinear optical signal in the molecular frame. The electric field emitted by the induced third-order polarization from impulsively pre-aligned gas-phase molecules at room temperature, in a degenerate four-wave mixing (DFWM) scheme, is measured using a spectral interferometry technique. We show that by measuring both the amplitude and phase of the emitted femtosecond pulse, information related to electronic symmetries can be accessed. The nonlinear signal is measured around a rotational revival to extract its molecular-frame angle dependence from pump-probe time delay scans. By comparing these measurements for two linear molecules, carbon dioxide (CO2) and Nitrogen (N2), we show that the measured second-order phase parameter (temporal chirp) of the signal is sensitive to the valence electronic symmetry of the molecules, whereas the amplitude of the signal does not show such sensitivity. We compare these measurements to theoretical calculations of the chirp observable in the molecular frame. This work is an important step towards using field-resolved nonlinear optical measurements to study ultrafast dynamics in electronically excited molecules.

physics.optics↗

arXiv2022

Electric Field Measurement of Femtosecond Time-Resolved Four-Wave Mixing Signals in Molecules

We report an experiment to measure the femtosecond electric field of the signal emitted from an optical third-order nonlinear interaction in carbon dioxide molecules. Using degenerate four-wave mixing with femtosecond near infrared laser pulses in combination with the ultra-weak femtosecond pulse measurement technique of TADPOLE, we measure the nonlinear signal electric field in the time domain at different time delays between the interacting pulses. The chirp extracted from the temporal phase of the emitted nonlinear signal is found to sensitively depend on the electronic and rotational contributions to the nonlinear response. While the rotational contribution results in a nonlinear signal chirp close to the chirp of the input pulses, the electronic contribution results in a significantly higher chirp which changes with time delay. Our work demonstrates that electric field-resolved nonlinear spectroscopy offers detailed information on nonlinear interactions at ultrafast time scales.

quant-ph↗