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Jens Biegert

Publications and source records attributed to Jens Biegert.

At least 19 recordsLinked to original sources

Chirally-sensitive optical rectification by isotropic chiral media

Chiroptical sensing is central to gain fundamental insight into electronic, vibrational and rotational degrees of freedom of chiral molecules, and is a cornerstone for nanomedicine and drug discovery platforms. Current chiral sensing technologies to assess the enantiomeric imbalance of chiral pharmaceutical compounds are sensitive to ml volumes but are time-consuming and cannot be integrated on a chip, thus creating a major bottleneck for drug discovery and nanomedicine. Here, we propose a novel chiroptical sensing approach based on optical rectification in a photonic micro-cavity filled by a drug solution with nl volume. We theoretically demonstrate that, upon optical excitation by intense pulsed laser light, such a nonlinear effect produces a chirally-sensitive nV voltage burst at the electrically-gated micro-cavity boundaries, with sign depending solely on the drug enantiomeric imbalance. Our results shed light on the potential of optical rectification as a robust platform for innovative lab-on-a-chip devices enabling chiral sensing with nl sensitivity.

physics.optics

Roadmap on Attosecond Science

Twenty-five years have passed since the first experimental demonstration of attosecond pulses, marking the advent of our ability to resolve and control electron motion in real time. What began as a technological breakthrough - generating the shortest flashes ever produced - has evolved into a powerful approach for probing and steering electronic dynamics in atoms, molecules, and solids. This roadmap, authored by leading experts in the field, surveys the recent rapid progress in the generation and characterization of attosecond pulses, emerging attosecond measurement and control techniques, and their expanding range of applications. It reviews current and future developments in attosecond light sources, including novel laser technologies, waveform synthesizers, new schemes for high-order harmonic generation, attosecond pulse generation at free-electron lasers, and structured light. Advances in attosecond measurement methodologies are also discussed, encompassing all-attosecond pump-probe spectroscopy, attosecond four-wave mixing, attosecond microscopy, spectroscopy with light transients, and attosecond interferometry. Furthermore, the roadmap addresses applications of attosecond spectroscopy to reveal electron dynamics in molecules and condensed matter systems from both theoretical and experimental perspectives, and highlights emerging directions at the interface with quantum optics and quantum entanglement. Overall, this work aims to serve as a comprehensive resource for navigating the evolving landscape of attosecond science.

physics.optics

Reply to "Comment on Brilliant source of 19.2 attosecond soft X-ray pulses below the atomic unit of time" by Han (arXiv:2510.17949)

We recently reported a refine analysis of a previously conducted soft X-ray (SXR) attosecond streaking measurement [1], employing the Variational Phase Gradient Temporal Analysis (VPGTA) retreival algorithm [2]. This re-evaluation, prompted by new metrological insights, revealed a 19.2 attosecond pulse - consistent with the expectations and estimates of our earlier work [3]. Shortly thereafter, a comment by M. Han [4] challenged our findings, citing "physical and technical issues concerning the original experiment and the new characterisation" inclusing purported contributions from Auger electrons, unfiltered low-energy harmonics, and uncompensated intrinsic chirp. These concerns, however, stem from misinterpretation of the experimental regime, selective citation of context, and disregard for well-established results in the peer-reviewed literature. In this reply, we address and clarify these points, demonstrating that the issues raised are not relevant under our experimental conditions. Given the highly specialized nature of attosecond genertaion and metrology in the soft X-ray water-window regime, we consider it essential to clarify these aspects of different regimes and reaffirm teh validity of our conclusions.

physics.optics

Brilliant source of 19.2 attosecond soft X-ray pulses below the atomic unit of time

Electronic correlations occur on attosecond timescales, dictating how chemical bonds form, energy flows, and materials respond to light. Capturing such many-body processes requires light pulses of similar duration. The soft X-ray water window is vital because it encompasses the principle absorption edges of carbon, nitrogen, and oxygen that underpin chemistry, biology, and materials science. However, generating and characterising isolated attosecond pulses that reach into the soft X-ray water window has remained a challenge. We addressed this need and report an isolated attosecond soft X-ray pulse with a duration of 19.2 attoseconds. This pulse reaches into the water window and is shorter than the atomic unit of time (24.2 as). The pulse is supported by a spectrum centred at 243 eV, extending up to 390 eV, and crossing the carbon K-edge with record photon flux: 4.8x10$^10$ photons per second overall and 4.1x10$^9$ photons per second in a 10% bandwidth at the carbon K-shell edge (284 eV). Such an extremely short soft X-ray pulse combines extreme temporal resolution with a coherent ultrabroadband soft X-ray spectrum, opening new opportunities to study electron dynamics in atoms, molecules, and solids, disentangle many-body interactions in correlated systems, and follow non-adiabatic energy flow in molecular complexes. Our results establish a new benchmark for table-top attosecond technology and lay the foundation for its widespread application in science and technology.

physics.optics

Revealing the anisotropic charge-density-wave order of TiSe$_2$ through high harmonic generation

Titanium diselenide (TiSe$_{2}$) is a transition-metal dichalcogenide material that undergoes a charge-density-wave (CDW) transition at $T_{c}\approx 200\,\mathrm{K}$. In a recent experiment [I. Tyulnev {\it et al.}, Commun. Mater. 6, 152 (2025)], the high harmonic generation (HHG) spectra of this material has been studied, which exhibits asymmetric behavior with respect to the polarization angle of the incident light and provides a new perspective to the CDW phase transition. In this work, we work out a theoretical explanation for the experimentally observed behavior of HHG spectra. We propose a simplified phenomenological mean-field model for this material, based on which the HHG spectra is calculated through the time-dependent Schr{\" o}dinger equation. This model correctly describes the measured intensity distribution of the third-, fifth-, and seventh-order harmonic generation as a function of polarization direction and reveals a strong asymmetry due to the anisotropic CDW order in the low temperature phase. Our work provides a basis for applying high harmonic spectroscopy to reveal a new perspective on the nature of CDW orders.

cond-mat.str-el

High harmonic spectroscopy reveals anisotropy of the Mott to Charge-Density-Wave phase transition in TiSe$_2$

This work explores the use of polarization-resolved high harmonic generation (HHG) spectroscopy to investigate the quantum phases and transitions in the correlated charge density wave (CDW) phase of TiSe$_2$. Unlike previous studies focusing on crystallographic changes, the research examines the reordering that occurs within the CDW phase as the material is cooled from room temperature to 14 K. By linking ultrafast field-driven dynamics to the material's potential landscape, the study demonstrates how HHG is sensitive to quantum phase transitions. The findings reveal an anisotropic component below the CDW transition temperature, providing new insights into the nature of this phase. The investigation highlights the interplay between linear and nonlinear optical responses and their departure from simple perturbative dynamics, offering a fresh perspective on correlated quantum phases in condensed matter systems.

cond-mat.str-el

Mid-Infrared Hyperspectral Microscopy with Broadband 1-GHz Dual Frequency Combs

Mid-infrared microscopy is an important tool for biological analyses, allowing a direct probe of molecular bonds in their low energy landscape. In addition to the label-free extraction of spectroscopic information, the application of broadband sources can provide a third dimension of chemical specificity. However, to enable widespread deployment, mid-infrared microscopy platforms need to be compact and robust while offering high speed, broad bandwidth and high signal-to-noise ratio (SNR). In this study, we experimentally showcase the integration of a broadband, high-repetition-rate dual-comb spectrometer (DCS) in the mid-infrared range with a scanning microscope. We employ a set of 1-GHz mid-infrared frequency combs, demonstrating their capability for high-speed and broadband hyperspectral imaging of polymers and ovarian tissue. The system covers 1000 $\mathrm{cm^{-1}}$ at $\mathrm{\nu_c=2941 \; cm^{-1}}$ with 12.86 kHz spectra acquisition rate and 5 $\mathrm{\mu m}$ spatial resolution. Taken together, our experiments and analysis elucidate the trade-off between bandwidth and speed in DCS as it relates to microscopy. This provides a roadmap for the future advancement and application of high-repetition-rate DCS hyperspectral imaging.

physics.optics

Evidence of the quantum-optical nature of high-harmonic generation

High-harmonic generation is a light up-conversion process occurring in a strong laser field, leading to coherent bursts of extreme ultrashort broadband radiation [1]. As a new perspective, we propose that ultrafast strong-field electronic or photonic processes such as high-harmonic generation can potentially generate non-classical states of light well before the decoherence of the system occurs [2, 3]. This could address fundamental challenges in quantum technology such as scalability, decoherence or the generation of massively entangled states [4]. Here, we report experimental evidence of the non-classical nature of the harmonic emission in several semiconductors excited by a femtosecond infrared laser. By investigating single- and double beam intensity cross-correlation [5], we measure characteristic, non-classical features in the single photon statistics. We observe two-mode squeezing in the generated harmonic radiation, which depends on the laser intensity that governs the transition from Super-Poissonian to Poissonian photon statistics. The measured violation of the Cauchy-Schwarz inequality realizes a direct test of multipartite entanglement in high-harmonic generation [6]. This result is supported by the theory of multimodal detection and the Hamiltonian from which the effective squeezing modes of the harmonics can be derived [7, 8]. With this work, we show experimentally that high-harmonic generation is a new quantum bosonic platform that intrinsically produces non-classical states of light with unique features such as multipartite broadband entanglement or multimode squeezing. The source operates at room temperature using standard semiconductors and a standard commercial fiber laser, opening new routes for the quantum industry, such as optical quantum computing, communication and imaging.

quant-ph

Valleytronics in bulk MoS$_2$ by optical control of parity and time symmetries

The valley degree of freedom of electrons in materials promises routes toward energy-efficient information storage with enticing prospects towards quantum information processing. Current challenges in utilizing valley polarization are symmetry conditions that require monolayer structures or specific material engineering, non-resonant optical control to avoid energy dissipation, and the ability to switch valley polarization at optical speed. We demonstrate all-optical and non-resonant control over valley polarization using bulk MoS$_2$, a centrosymmetric material with zero Berry curvature at the valleys. Our universal method utilizes spin-angular momentum-shaped tri-foil optical control pulses to switch the material's electronic topology to induce valley polarization by transiently breaking time and space inversion symmetry through a simple phase rotation. The dependence of the generation of the second harmonic of an optical probe pulse on the phase rotation directly demonstrates the efficacy of valley polarization. It shows that direct optical control over the valley degree of freedom is not limited to monolayer structures. Instead, it is possible for systems with an arbitrary number of layers and bulk materials. Universal and non-resonant valley control at optical speeds unlocks the possibility of engineering efficient, multi-material valleytronic devices operating on quantum coherent timescales.

cond-mat.mtrl-sci

Theory of X-ray absorption spectroscopy: a microscopic Bloch equation approach for two-dimensional solid states

We develop a self-consistent Maxwell-Bloch formalism for the interaction of X-rays with two-dimensional crystalline materials by incorporating the Bloch theorem and Coulomb many-body interaction. This formalism is illustrated for graphene, by calculating the polarization-dependent XANES, formulating expressions for the radiative and Meinter-Auger recombination of core-holes, and the discussion of microscopic insights into the spectral oscillations of EXAFS beyond point scattering theory. In particular, the correct inclusion of lattice periodicity in our evaluation allows us to assign so far uninterpreted spectral features in the Fourier transformed EXAFS spectrum.

cond-mat.mes-hall

High harmonic spectroscopy of quantum phase transitions in a high-T$_c$ superconductor

We report on the new non--linear optical signatures of quantum phase transitions in the high-temperature superconductor YBCO, observed through high harmonic generation. While the linear optical response of the material is largely unchanged when cooling across the phase transitions, the nonlinear optical response sensitively imprints two critical points, one at the critical temperature of the cuprate with the exponential growth of the surface harmonic yield in the superconducting phase, and another critical point, which marks the transition from strange metal to pseudo gap phase. To reveal the underlying microscopic quantum dynamics, a novel strong-field quasi-Hubbard model was developed, which describes the measured optical response dependent on the formation of Cooper pairs. Further, the new theory provides insight into the carrier scattering dynamics and allows to differentiate between the superconducting, pseudo gap, and strange metal phases. The direct connection between non--linear optical response and microscopic dynamics provides a powerful new methodology to study quantum phase transitions in correlated materials. Further implications are light-wave control over intricate quantum phases, light-matter hybrids, and application for optical quantum computing.

cond-mat.supr-con

Machine learning for laser-induced electron diffraction imaging of molecular structures

Ultrafast diffraction imaging is a powerful tool to retrieve the geometric structure of gas-phase molecules with combined picometre spatial and attosecond temporal resolution. However, structural retrieval becomes progressively difficult with increasing structural complexity, given that a global extremum must be found in a multi-dimensional solution space. Worse, pre-calculating many thousands of molecular configurations for all orientations becomes simply intractable. As a remedy, here, we propose a machine learning algorithm with a convolutional neural network which can be trained with a limited set of molecular configurations. We demonstrate structural retrieval of a complex and large molecule, Fenchone (C$_{10}$H$_{16}$O), from laser-induced electron diffraction (LIED) data without fitting algorithms or ab initio calculations. Retrieval of such a large molecular structure is not possible with other variants of LIED or ultrafast electron diffraction. Combining electron diffraction with machine learning presents new opportunities to image complex and larger molecules in static and time-resolved studies.

physics.chem-ph

Generating high density molecular jets of complex neutral organic molecules using micro-sized Tesla valves

We report the design and implementation of multiple Tesla type micro valves in the target delivery system of a reaction microscope (ReMi) to study gas phase structural dynamics of complex polyatomic molecules, when no delivery system currently exists that can deliver dense enough molecular jets of neutral complex molecules without ionizing or exciting the target. We show, the Tesla valves provide an efficient unidirectional flow of the cis-stilbene molecules into the ReMi. We demonstrate using a bubbler with Tesla valves an order-of-magnitude increase in the detected stilbene molecular ion signal following the strong-field tunnel ionization (SFTI), compared to conventional bubbler without any Tesla valves. Our results for the first time, opens the door for studying large, complex neutral molecules in the gas-phase with low vapour pressures in future ultrafast studies.

physics.atom-ph

Laser-induced electron diffraction of the ultrafast umbrella motion in ammonia

Visualizing molecular transformations in real-time requires a structural retrieval method with Ångström spatial and femtosecond temporal atomic resolution. Imaging of hydrogen-containing molecules additionally requires an imaging method that is sensitive to the atomic positions of hydrogen nuclei, with most methods possessing relatively low sensitivity to hydrogen scattering. Laser-induced electron diffraction (LIED) is a table top technique that can image ultrafast structural changes of gas-phase polyatomic molecules with sub-Ångström and femtosecond spatiotemporal resolution together with relatively high sensitivity to hydrogen scattering. Here, we image the umbrella motion of an isolated ammonia molecule (NH$_3$) following its strong field ionization. Upon ionization of a neutral ammonia molecule, the ammonia cation (NH$_3^+$) undergoes an ultrafast geometrical transformation from a pyramidal ($Φ_{HNH} = 107 ^\circ$) to planar ($Φ_{HNH}=120^\circ$) structure in approximately 8 femtoseconds. Using LIED, we retrieve a near-planar ($Φ_{HNH}=117 \pm 5^\circ$) field-dressed NH$_3^+$ molecular structure $7.8-9.8$ femtoseconds after ionization. Our measured field-dressed NH$_3^+$ structure is in excellent agreement with our calculated equilibrium field dressed structure using quantum chemical ab initio calculations.

physics.chem-ph

High-brightness seven-octave carrier envelope phase-stable light source

High-brightness sources of coherent and few-cycle-duration light waveforms with spectral coverage from the UV to the THz would offer unprecedented versatility and opportunities for a spectacular range of applications from bio-chemical sensing, to time-resolved and nonlinear spectroscopy, to attosecond light-wave electronics. Combinations of various sources with frequency conversion and supercontinuum generation can provide relatively large spectral coverage, but many applications require much broader spectral range and low-jitter synchronization for time-domain measurements. Here, we present a carrier-envelope-phase stable light source, seeded by a mid-IR frequency comb, with simultaneous spectral coverage across 7 optical octaves, from the UV (340 nm) into the THz (40,000 nm). Combining soliton self-compression and dispersive wave generation in an anti-resonant-reflection photonic crystal fibre with intra-pulse difference frequency generation in BaGa2GeSe6, the spectral brightness is 2-5 orders of magnitude above synchrotron sources. This enables high-dynamic-range spectroscopies and provides enticing prospects for attosecond physics and material sciences.

physics.optics

Attosecond state-resolved carrier motion in quantum materials probed by soft X-ray XANES

Recent developments in attosecond technology led to tabletop X-ray spectroscopy in the soft X-ray range, thus uniting the element- and state-specificity of core-level x-ray absorption spectroscopy with the time resolution to follow electronic dynamics in real time. We describe recent work in attosecond technology and investigations into materials such as Si, SiO2, GaN, Al2O3, Ti, TiO2, enabled by the convergence of these two capabilities. We showcase the state-of-the-art on isolated attosecond soft x-ray pulses for x-ray absorption near edge spectroscopy (XANES) to observe the 3d-state dynamics of the semi-metal TiS2 with attosecond resolution at the Ti L-edge (460 eV). We describe how the element- and state-specificity at the transition metal L-edge of the quantum material allows to unambiguously identify how and where the optical field influences charge carriers. This precision elucidates that the Ti:3d conduction band states are efficiently photo-doped to a density of 1.9 x 10^21 cm^-3 and that the light-field induces coherent motion of intra-band carriers across 38% of the first Brillouin zone. Lastly, we describe the prospects with such unambiguous real-time observation of carrier dynamics in specific bonding or anti-bonding states and speculate that such capability will bring unprecedented opportunities towards an engineered approach for designer materials with pre-defined properties and efficiency. Examples are composites of semiconductors and insulators like Si, Ge, SiO2, GaN, BN, quantum materials like graphene, TMDCs, or high-Tc superconductors like NbN or LaBaCuO. Exiting are prospects to scrutinize canonical questions in multi-body physics such as whether the electrons or lattice trigger phase transitions.

cond-mat.mtrl-sci

Symphony on Strong Field Approximation

This paper has been prepared by the Symphony collaboration (University of Warsaw, Uniwersytet Jagielloński, DESY/CNR and ICFO) on the occasion of the 25th anniversary of the "simple man's models" which underlie most of the phenomena that occur when intense ultrashort laser pulses interact with matter. The phenomena in question include High-Harmonic Generation, Above-Threshold Ionization, and Non-Sequential Multielectron Ionization. "Simple man's models" provide, both an intuitive basis for understanding the numerical solutions of the time-dependent Schrödinger equation, and the motivation for the powerful analytic approximations generally known as the Strong Field Approximation (SFA). In this paper we first review the SFA in the form developed by us in the last 25 years. In this approach SFA is a method to solve the TDSE using a systematic perturbation theory in a part of the Hamiltonian describing continuum-continuum transitions in the presence of the laser field. In this review we focus on recent applications of SFA to HHG, ATI and NSMI from multi-electron atoms and from multi-atom. The main novel part of the presented theory concerns generalizations of SFA to: (i) time-dependent treatment of two-electron atoms, allowing for studies of an interplay between Electron Impact Ionization (EII) and Resonant Excitation with Subsequent Ionization (RESI); (ii) time-dependent treatment in the single active electron (SAE) approximation of "large" molecules and targets which are themselves undergoing dynamics during the HHG or ATI process. In particular, we formulate the general expressions for the case of arbitrary molecules, combining input from quantum chemistry and quantum dynamics. We formulate also theory of time-dependent separable molecular potentials to model analytically the dynamics of realistic electronic wave packets for molecules in strong laser fields.

quant-ph