arXiv subjects

Lorenz Drescher

Publications and source records attributed to Lorenz Drescher.

7 recordsLinked to original sources

arXiv2024

Attosecond transient grating spectroscopy with near-infrared grating pulses and an extreme ultraviolet diffracted probe

Transient grating spectroscopy has become a mainstay among metal and semiconductor characterization techniques. Here we extend the technique towards the shortest achievable timescales by using tabletop high-harmonic generation of attosecond extreme ultraviolet (XUV) pulses that diffract from transient gratings generated with 500-1000 nm sub-5 fs near-infrared (NIR) pulses. We demonstrate the power of attosecond transient grating spectroscopy (ATGS) by investigating the ultrafast photoexcited dynamics in an Sb semimetal thin film. ATGS provides an element-specific, background-free signal, unfettered by spectral congestion, in contrast to transient absorption spectroscopy. With the ATGS measurements in Sb polycrystalline thin films, we observe the generation of coherent phonons and investigate the lattice and carrier dynamics. Among the latter processes, we extract carrier thermalization, hot carrier cooling, and electron-hole recombination, which are on the order of 20 fs, 50 fs, and 2 ps, timescales, respectively. Furthermore, simultaneous collection of transient absorption and transient grating data allows us to extract the total complex dielectric constant in the sample dynamics, including the real-valued refractive index, from which we are also able to investigate carrier-phonon interactions and longer-lived phonon dynamics. The outlined experimental technique expands the capabilities of transient grating spectroscopy and attosecond spectroscopies by providing a wealth of information concerning carrier and lattice dynamics with an element-selective technique, at the shortest achievable timescales.

physics.optics↗

arXiv2024

Initial electron thermalization in metals measured by attosecond transient absorption spectroscopy

Understanding initial electron thermalization has relevance to both fundamental scientific knowledge and application to the construction of novel devices. In this study, attosecond transient absorption is used to directly measure initial electron thermalization times of 38 $\pm$ 8 fs, 15 $\pm$ 3 fs, 4.2 $\pm$ 1 fs, and 2.0 $\pm$ 0.3 fs for Mg, Pt, Fe, and Co, respectively. Through time dependent density function theory calculations, it is shown that the fast electron thermalization observed in Fe and Co is correlated with a strong local field effect. We find that a simple analytical model can be used to calculate the initial electron thermalization time measured by the transient extreme ultraviolet absorption spectroscopy method performed here. Our results suggest that the most significant contributions to the initial electron thermalization times are the basic metal properties of the density of states volume available for scattering and screened electron interaction. Many-body effects contribute less, but still significantly to the initial electron thermalization time. Ultimately the information gained through this study shows the unique view that attosecond transient absorption spectroscopy contributes to unraveling and monitoring electron dynamics and its connection to many-body effects in metals and beyond.

cond-mat.mtrl-sci↗

arXiv2021

Phase-Dependence of Resonant and Antiresonant Two-Photon Excitations

Measurements of the phase of two-photon matrix elements are presented for resonant and antiresonant two-color ionization of helium. A tunable, narrow-bandwidth, near-infrared (NIR) laser source is used for extreme ultra-violet (XUV) high-harmonic generation (HHG). The 15th harmonic of the laser is used within (1+1') XUV+NIR two-photon ionization, and tuned in and out of resonance with members of the 1s$n$p $^1$P$_1$ ($n=3,4,5$) Rydberg series, covering a broad spectral range with high spectral resolution. The technique allows to observe characteristic rapid changes in the phase of the two-photon matrix elements around the resonances and, previously unobserved, at the antiresonances between the resonances. Similar effects are observed for (1+2') XUV+NIR three-photon ionization. The experimental results are compared to a perturbative model and to numerical solutions of the time-dependent Schrödinger equation (TDSE) in the single active electron (SAE) approximation, elucidating the origin and dependences of the observed phenomena.

physics.atom-ph↗

arXiv2021

Experimental control of quantum-mechanical entanglement in an attosecond pump-probe experiment

Entanglement is one of the most intriguing aspects of quantum mechanics and lies at the heart of the ongoing Second Quantum Revolution, where it is a resource that is used in quantum key distribution, quantum computing and quantum teleportation. We report experiments demonstrating the crucial role that entanglement plays in pump-probe experiments involving ionization, which are a hallmark of the novel research field of attosecond science. We demonstrate that the degree of entanglement in a bipartite ion plus photoelectron system, and, as a consequence, the degree of vibrational coherence in the ion, can be controlled by tailoring the spectral properties of the attosecond extreme ultra-violet laser pulses that are used to create them.

quant-ph↗

arXiv2021

Vibrational relaxation of hot ground state cations of naphthalene

Time-resolved XUV-IR photoion mass spectroscopy of naphthalene conducted with broadband, as well as with wavelength-selected narrowband XUV pulses reveals a rising probability of fragmentation characterized by a lifetime of $92\pm4$~fs. This lifetime is independent of the XUV excitation wavelength and is the same for all low appearance energy fragments recorded in the experiment. Analysis of the experimental data in conjunction with a statistical multi-state vibronic model suggests that the experimental signals track vibrational energy redistribution on the potential energy surface of the ground state cation. In particular, populations of the out-of-plane ring twist and the out-of-plane wave bending modes could be responsible for opening new IR absorption channels leading to enhanced fragmentation.

physics.chem-ph↗

arXiv2020

Attosecond Transient Absorption Spectroscopy without Inversion Symmetry

Transient absorption is a very powerful observable in attosecond experiments on atoms, molecules and solids and is frequently used in experiments employing phase-locked few-cycle infrared and XUV laser pulses derived from high harmonic generation. We show numerically and analytically that in non-centrosymmetric systems, such as many polyatomic molecules, which-way interference enabled by the lack of parity conservation leads to new spectral absorption features, which directly reveal the laser electric field. The extension of Attosecond Transient Absorption Spectroscopy (ATAS) to such targets hence becomes sensitive to global and local inversion symmetry. We anticipate that ATAS will find new applications in non-centrosymmetric systems, in which the carrier-to-envelope phase of the infrared pulse becomes a relevant parameter and in which the orientation of the sample and the electronic symmetry of the molecule can be addressed.

physics.atom-ph↗

arXiv2018

Extreme-ultraviolet refractive optics

Refraction is a well-known optical phenomenon that alters the direction of light waves propagating through matter. Microscopes, lenses and prisms based on refraction are indispensable tools for controlling the properties of light beams at visible, infrared, ultraviolet and X-ray wavelengths. The large absorption of extreme-ultraviolet (XUV) radiation in matter, however, hinders the development of refractive lenses and prisms in this spectral region. Here, we demonstrate control over the refraction of XUV radiation by using a gas jet with a density gradient across the XUV beam profile. A gas phase prism is demonstrated that leads to a frequency-dependent deflection of the XUV beam. The strong deflection in the vicinity of atomic resonances is further used to develop a deformable XUV refractive lens, with low absorption and a focal length that can be tuned by varying the gas pressure. Our results provide novel opportunities in XUV science and open a route towards the transfer of refraction-based techniques including microscopy and nanofocusing, which are well established in other spectral regions, to the XUV domain.

physics.optics↗