Petahertz electronics

Abstract Measuring transient optical fields is pivotal not only for understanding ultrafast phenomena but also for the quantitative detection of various molecular species in a sample. Here we demonstrate near-petahertz electric field detection of a few femtosecond pulses with 200 attosecond temporal resolution and subfemtojoule detection sensitivity. By field-resolved detection of the impulsively excited molecules in the liquid phase, termed femtosecond fieldoscopy, we demonstrate temporal isolation of the response of the target molecules from those of the environment and the excitation pulse. In a proof-of-concept analysis of aqueous and liquid samples, we demonstrate field-sensitive detection of combination bands of 4.13 μmol ethanol for the first time. This method expands the scope of aqueous sample analysis to higher detection sensitivity and dynamic range, while the simultaneous direct measurements of phase and intensity information pave the path towards high-resolution biological spectro-microscopy. 

pdf/near-petahertz-fieldoscopy-of-liquid-1wb37gqdd2jp.pdf

Near-petahertz fieldoscopy of liquid

We demonstrate sensitive electric field measurements by coherent homodyne amplification of the electric field induced second harmonic generation (E-FISH) technique. In the process of E-FISH, an applied electric field breaks the centrosymmetry of an otherwise homogeneous medium, in turn promoting the generation of the second harmonic frequency of an incident field. Due to weak third-order hyperpolarizability and the requirement of an applied field to break the symmetry, the E-FISH technique has been mainly used to study high fields, also requiring a strong optical field and sensitive detection. Here we superimpose the E-FISH signal with an auxiliary beam, also termed a local oscillator (LO), at double the incident frequency. Coherent superposition of the LO and the E-FISH output (LOE-FISH) allows for a homodyne amplification of the otherwise weak nonlinear signal. We have demonstrated an increase of signal-to-noise by a factor of seven, which results in a measurement time reduction of a factor of 49. This technique, LOE-FISH, has a number of advantages: detection with intensified detectors is not required. Furthermore, instead of millijoule pulsed lasers, we can work with microjoule pulsed lasers, which allows measuring at repetition rates of megahertz and opens single shot and real-time capability. The LOE-FISH technique increases in sensitivity at lower electric field values. Our work is a demonstration of the principle. Already with our first results from the demonstration, one can see the high potential of LOE-FISH. 

Sensitive detection of electric field-induced second harmonic signals.

Time-domain analysis of harmonic fields with sub-cycle resolution is now experimentally viable due to the emergence of sensitive, on-chip techniques for petahertz-scale optical-field sampling. We demonstrate how such a time-domain, field-resolved analysis uncovers the extreme nonlinear electron dynamics responsible for high-harmonic generation within solids. Time-dependent density functional theory was used to simulate harmonic generation from a solid-state band-gap system driven by near- to mid-infrared waveforms. Particular attention was paid to regimes where both intraband and interband emission mechanisms play a critical role in shaping the nonlinear response. We show that a time-domain analysis of the harmonic radiation fields identifies the interplay between intra- and interband dynamical processes underlying the nonlinear light generation. With further analysis, we show that changes to the dominant emission regime can occur after only slight changes to the peak driving intensity and central driving wavelength. Time-domain analysis of harmonic fields also reveals, for the first time, the possibility of rapid changes in the dominant emission mechanism within the temporal window of the driving pulse envelope. Finally, we examine the experimental viability of performing time-domain analysis of harmonic fields with sub-cycle resolution using realistic parameters. 

/pdf/uncovering-extreme-nonlinear-dynamics-in-solids-through-time-3769fwvs.pdf

Uncovering extreme nonlinear dynamics in solids through time-domain field analysis

Measuring an electric field waveform beyond radio frequencies is often accomplished via a second-order nonlinear interaction with a laser pulse shorter than half of the field's oscillation period. However, synthesizing such a gate pulse is extremely challenging when sampling mid- (MIR) and near- (NIR) infrared transients. Here, we demonstrate an alternative approach: a third-order nonlinear interaction with a relatively long multi-cycle pulse directly retrieves an electric-field transient whose central frequency is 156 THz. A theoretical model, exploring the different nonlinear frequency mixing processes, accurately reproduces our results. Furthermore, we demonstrate a measurement of the real part of a sample's dielectric function, information that is challenging to retrieve in time-resolved spectroscopy and is therefore often overlooked. The new method paves the way towards experimentally simple MIR-to-NIR time-resolved spectroscopy that simultaneously extracts the spectral amplitude and phase information, an important extension of optical pump-probe spectroscopy of, e.g., molecular vibrations and fundamental excitations in condensed-matter physics. 

https://www.nature.com/articles/s42005-023-01269-y.pdf

Few-femtosecond phase-sensitive detection of infrared electric fields with a third-order nonlinearity

The ability to resolve the complete electric field of laser pulses from terahertz to mid-infrared spectral ranges has enriched time-domain spectroscopy for decades. Field-resolved measurements in this range have been performed routinely in ambient air by various techniques like electro-optic sampling, photoconductive switching, field-induced second harmonic generation, and time stretch photonics. On the contrary, resolving the electric field of light at the near-infrared spectral range has been limited to attosecond streaking and other techniques that require operation in vacuum. Recent advances are circumventing these shortcomings and extending the direct, ambient air field detection of light to petahertz frequencies. In the first part of this letter, recent field-resolved techniques are reviewed. In the second part, different approaches for temporal scanning are discussed, as the temporal resolution of the time-domain methods is prone to temporal jitter. The review concludes by discussing technological obstacles and emerging applications of such advancements.

https://iopscience.iop.org/article/10.1088/1361-6455/ac8032/pdf

Recent advances in petahertz electric field sampling

Ultrashort time-domain spectroscopy and field-resolved spectroscopy of molecular fingerprints are gold standards for detecting samples’ constituents and internal dynamics. However, they are hindered by the Nyquist criterion, leading to prolonged data acquisition, processing times, and sizable data volumes. In this work, we present the first experimental demonstration of compressed sensing on field-resolved molecular fingerprinting by employing random scanning. Our measurements enable pinpointing the primary absorption peaks of atmospheric water vapor in response to terahertz light transients while sampling beyond the Nyquist limit. By drastically undersampling the electric field of the molecular response at a Nyquist frequency of 0.8 THz, we could successfully identify water absorption peaks up to 2.5 THz with a mean squared error of 12 × 10 −4 . To our knowledge, this is the first experimental demonstration of time-domain compressed sensing, paving the path toward real-time field-resolved fingerprinting and acceleration of advanced spectroscopic techniques. 

Compressed Sensing of Field-resolved Molecular Fingerprint Beyond the Nyquist Frequency

Abstract Understanding the photodamage mechanism underlying the highly nonlinear dynamic of femtosecond laser pulses at the second transparent window of tissue is crucial for label-free microscopy. Here, we report the identification of two cavitation regimes from 1030 nm pulses when interacting with the central nervous system in zebrafish. We show that at low repetition rates, the damage is confined due to plasma-based ablation and sudden local temperature rise. At high repetition rates, the damage becomes collateral due to plasma-mediated photochemistry. Furthermore, we investigate the role of fluorescence labels with linear and nonlinear absorption pathways in optical breakdown. To verify our findings, we examined cell death and cellular responses to tissue damage, including the recruitment of fibroblasts and immune cells after irradiation. These findings contribute to advancing the emerging nonlinear optical microscopy techniques and provide a strategy for inducing precise, and localized injuries using near-infrared femtosecond laser pulses. 

pdf/nonlinear-dynamics-of-femtosecond-laser-interaction-with-the-5fq3b8f8q7.pdf

Nonlinear dynamics of femtosecond laser interaction with the central nervous system in zebrafish

We propose a concept for Raman distributed temperature sensing based on L-band excitation and C-band Anti-Stokes detection. The concept is demonstrated by interrogation of 1500 m fiber with incoherent optical frequency domain reflectometry.

Concept for Raman Distributed Temperature Sensing in Optical Fibers based on Standard C-Band Spectrometer

Octave-spanning, field-resolved, Kerr-amplification in liquid thin film

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