Leitenstorfer, Alfred
0000-0002-9847-257X Berufsbeschreibung
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Few-femtosecond phase-sensitive detection of infrared electric fields with a third-order nonlinearity
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. Our 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.
The 2023 terahertz science and technology roadmap
Terahertz (THz) radiation encompasses a wide spectral range within the electromagnetic spectrum that extends from microwaves to the far infrared (100 GHz–∼30 THz). Within its frequency boundaries exist a broad variety of scientific disciplines that have presented, and continue to present, technical challenges to researchers. During the past 50 years, for instance, the demands of the scientific community have substantially evolved and with a need for advanced instrumentation to support radio astronomy, Earth observation, weather forecasting, security imaging, telecommunications, non-destructive device testing and much more. Furthermore, applications have required an emergence of technology from the laboratory environment to production-scale supply and in-the-field deployments ranging from harsh ground-based locations to deep space. In addressing these requirements, the research and development community has advanced related technology and bridged the transition between electronics and photonics that high frequency operation demands. The multidisciplinary nature of THz work was our stimulus for creating the 2017 THz Science and Technology Roadmap (Dhillon et al 2017 J. Phys. D: Appl. Phys. 50 043001). As one might envisage, though, there remains much to explore both scientifically and technically and the field has continued to develop and expand rapidly. It is timely, therefore, to revise our previous roadmap and in this 2023 version we both provide an update on key developments in established technical areas that have important scientific and public benefit, and highlight new and emerging areas that show particular promise. The developments that we describe thus span from fundamental scientific research, such as THz astronomy and the emergent area of THz quantum optics, to highly applied and commercially and societally impactful subjects that include 6G THz communications, medical imaging, and climate monitoring and prediction. Our Roadmap vision draws upon the expertise and perspective of multiple international specialists that together provide an overview of past developments and the likely challenges facing the field of THz science and technology in future decades. The document is written in a form that is accessible to policy makers who wish to gain an overview of the current state of the THz art, and for the non-specialist and curious who wish to understand available technology and challenges. A such, our experts deliver a ‘snapshot’ introduction to the current status of the field and provide suggestions for exciting future technical development directions. Ultimately, we intend the Roadmap to portray the advantages and benefits of the THz domain and to stimulate further exploration of the field in support of scientific research and commercial realisation.
Passively phase-locked Er:fiber source of single-cycle pulses in the near infrared with electro-optic timing modulation for field-resolved electron control
A single-cycle light source in the near infrared is demonstrated enabling sensitive applications of ultrafast optical field control of electronic transport. The compact Er:fiber system generates passively phase-locked pulses with broadband spectra covering 150 THz to 350 THz at a duration of 4.2 fs and 40 MHz repetition rate. A second output arm is equipped with an electro-optic modulator that switches the arrival time of the pulses by 700 ps at arbitrary frequencies up to 20 MHz, enabling timing modulation of the pump pulse without changing the average intensity. As a benchmark demonstration, we investigate the carrier relaxation dynamics in low-temperature-grown InGaAs using quantum interference currents.
Realizing a rapidly switched Unruh-DeWitt detector through electro-optic sampling of the electromagnetic vacuum
A new theoretical framework to describe the experimental advances in electro-optic detection of broadband quantum states, specifically the quantum vacuum, is devised. Electro-optic sampling is a technique in ultrafast photonics which, when transferred into the quantum domain, can be utilized to resolve properties of a sampled quantum state via its interaction with a strong coherent probe pulse at ultrafast timescales. By making use of fundamental concepts from quantum field theory on spacetime metrics, the nonlinear interaction behind the electro-optic effect is shown to be equivalent to a stationary Unruh-DeWitt detector coupled to a conjugate field during a very short time interval. When the coupling lasts for a time interval comparable to the oscillation periods of the detected field mode (i.e., the subcycle regime), virtual particles inhabiting the field vacuum are transferred to the detector in the form of real excitation. We demonstrate that this behavior can be rigorously translated to the scenario of electro-optic sampling of the quantum vacuum, in which the (spectrally filtered) probe works as an Unruh-DeWitt detector, with its interaction-generated photons arising from virtual particles inhabiting the electromagnetic vacuum. Our analysis accurately encapsulates the quantum nature of the vacuum, and we propose the specific working regime in which we can experimentally verify the existence of virtual photons with quantum correlations in the electromagnetic ground state.
Dissection of DNA damage and repair pathways in live cells by femtosecond laser microirradiation and free-electron modeling
Understanding and predicting the outcome of the interaction of light with DNA has a significant impact on the study of DNA repair and radiotherapy. We report on a combination of femtosecond pulsed laser microirradiation at different wavelengths, quantitative imaging, and numerical modeling that yields a comprehensive picture of photon-mediated and free-electron-mediated DNA damage pathways in live cells. Laser irradiation was performed under highly standardized conditions at four wavelengths between 515 nm and 1,030 nm, enabling to study two-photon photochemical and free-electron-mediated DNA damage in situ. We quantitatively assessed cyclobutane pyrimidine dimer (CPD) and γH2AX-specific immunofluorescence signals to calibrate the damage threshold dose at these wavelengths and performed a comparative analysis of the recruitment of DNA repair factors xeroderma pigmentosum complementation group C (XPC) and Nijmegen breakage syndrome 1 (Nbs1). Our results show that two-photon-induced photochemical CPD generation dominates at 515 nm, while electron-mediated damage dominates at wavelengths ≥620 nm. The recruitment analysis revealed a cross talk between nucleotide excision and homologous recombination DNA repair pathways at 515 nm. Numerical simulations predicted electron densities and electron energy spectra, which govern the yield functions of a variety of direct electron-mediated DNA damage pathways and of indirect damage by • OH radicals resulting from laser and electron interactions with water. Combining these data with information on free electron–DNA interactions gained in artificial systems, we provide a conceptual framework for the interpretation of the wavelength dependence of laser-induced DNA damage that may guide the selection of irradiation parameters in studies and applications that require the selective induction of DNA lesions.
Back action in quantum electro-optic sampling of electromagnetic vacuum fluctuations
The influence of measurement back action on electro-optic sampling of electromagnetic quantum fluctuations is investigated. Based on a cascaded treatment of the nonlinear interaction between a near-infrared coherent probe and the mid-infrared vacuum, we account for the generated electric-field contributions that lead to detectable back action. Specifically, we theoretically address two realistic setups, exploiting one or two probe beams for the nonlinear interaction with the quantum vacuum, respectively. The setup parameters at which back action starts to considerably contaminate the measured noise profiles are determined. We find that back action starts to detrimentally affect the signal once the fluctuations due to the coupling to the mid-infrared vacuum become comparable to the base shot noise. Due to the vacuum fluctuations entering at the beam splitter, the shot noise of two incoming probe pulses in different channels is uncorrelated. Therefore, even when the base shot noise dominates the output of the experiment, it does not contribute to the correlation signal itself. However, we find that further contributions due to nonlinear shot-noise enhancement are still present. Ultimately, a regime in which electro-optic sampling of quantum fields can be considered as effectively back-action free is found.
Quantitative analysis of free-electron dynamics in InSb by terahertz shockwave spectroscopy
The contribution of free electrons to the dielectric function is largely determined by their plasmonic resonance, a collective density oscillation. We studied this broadband and carrier-density-dependent response in the narrow-gap semiconductor InSb with THz shockwave spectroscopy. A synthesized waveform, with a steep onset followed by a short electric-field plateau, gives access to a multioctave spectrum of frequencies from 100 GHz up to the mid infrared. By measuring the entire spectral characteristics of the plasma, we analyze the dynamics of photogenerated free electrons for a wide range of excitation fluences. Thanks to this analysis, we were able to quantify the coefficients of both electron trapping and the Auger process from cryogenic to room temperature.
Femtosecond Frequency Combs with Few‐kHz Passive Stability over an Ultrabroadband Spectral Range
Femtosecond frequency combs are among the most precise measurement tools in existence. They have applications ranging from high-precision spectroscopy and metrology to time-domain quantum physics. Maximizing the passive stability of these instruments is essential to achieve their full potential in fundamental science and high-tech industry. However, the noise mechanisms across the entire operating space of these devices have not been fully characterized. Here the noise properties of fiber-based frequency combs are studied as a function of intracavity dispersion, pump power, and repetition rate. Distinct minima are discovered in this parameter space where the free-running linewidth of the carrier-envelope offset (CEO) frequency fCEO drops below 1 kHz. The individual comb lines are analyzed spread over a wide spectral range producing a complete understanding of the particular contributions to the phase noise and their interplay. Exploiting these findings, combs featuring sharp teeth at specific frequency positions and over the entire spectrum from fCEO to 300 THz are demonstrated. The ultrabroadband stability offered by these compact systems provides a new level of quality for front-end measurement tasks in both time and frequency domains.
Tracing attosecond electron emission from a nanometric metal tip
Solids exposed to intense electric fields release electrons through tunnelling. This fundamental quantum process lies at the heart of various applications, ranging from high brightness electron sources in d.c. operation1,2 to petahertz vacuum electronics in laser-driven operation3,4,5,6,7,8. In the latter process, the electron wavepacket undergoes semiclassical dynamics9,10 in the strong oscillating laser field, similar to strong-field and attosecond physics in the gas phase11,12. There, the subcycle electron dynamics has been determined with a stunning precision of tens of attoseconds13,14,15, but at solids the quantum dynamics including the emission time window has so far not been measured. Here we show that two-colour modulation spectroscopy of backscattering electrons16 uncovers the suboptical-cycle strong-field emission dynamics from nanostructures, with attosecond precision. In our experiment, photoelectron spectra of electrons emitted from a sharp metallic tip are measured as function of the relative phase between the two colours. Projecting the solution of the time-dependent Schrödinger equation onto classical trajectories relates phase-dependent signatures in the spectra to the emission dynamics and yields an emission duration of 710 ± 30 attoseconds by matching the quantum model to the experiment. Our results open the door to the quantitative timing and precise active control of strong-field photoemission from solid state and other systems and have direct ramifications for diverse fields such as ultrafast electron sources17, quantum degeneracy studies and sub-Poissonian electron beams18,19,20,21, nanoplasmonics22 and petahertz electronics23.
Quantum Susceptibilities in Time-Domain Sampling of Electric Field Fluctuations
Electro-optic sampling has emerged as a new quantum technique enabling measurements of electric field fluctuations on subcycle time scales. In a second-order nonlinear material, the fluctuations of a terahertz field are imprinted onto the polarization properties of an ultrashort probe pulse in the near infrared. The statistics of this time-domain signal are calculated, incorporating the quantum nature of the involved electric fields right from the beginning. A microscopic quantum theory of the electro-optic process is developed adopting an ensemble of noninteracting three-level systems as a model for the nonlinear material. It is found that the response of the nonlinear medium can be separated into a conventional part, which is exploited also in sampling of coherent amplitudes, and quantum contributions, which are independent of the state of the terahertz input. Interactions between the three-level systems which are mediated by terahertz vacuum fluctuations are causing this quantum response. Conditions under which the classical response serves as a good approximation of the electro-optic process are also determined and how the statistics of the sampled terahertz field can be reconstructed from the electro-optic signal is demonstrated. In a complementary regime, electro-optic sampling can serve as a spectroscopic tool to study the pure quantum susceptibilities of matter.