arXiv subjects

Christoph Lienau

Publications and source records attributed to Christoph Lienau.

At least 19 recordsLinked to original sources

arXiv2026

Coherent interaction of WS$_2$ and quasi-2D perovskite excitons over micrometer distances via a cavity field

The coherent coupling of cavity-confined photons and excitonic matter resonances leads to the formation of cavity polaritons, hybrid light-matter quasi-particles. If multiple exciton resonances couple to the same photonic mode, the resulting polariton constitutes a coherent interaction between matter resonances that can be spatially separated without any direct electronic coupling. In this work, we demonstrate the formation of such a coherent coupling at room temperature using an open optical cavity containing two distinct van der Waals materials - monolayer WS2 and layered quasi-2D halide perovskites (HaPs) - separated by $1.5 μ\rm m$. The system forms three polariton branches, with the middle branch possessing nearly equal fractions of both excitons and the photonic mode. White-light reflectivity and luminescence measurements are in good agreement with simulations using a coupled harmonic oscillator and a microscopic Wannier-Hopfield framework. Our results lay the foundation to combine highly complementary degrees of freedom in 2D materials in an in-situ tunable fashion to enable new polaritonic functionalities.

cond-mat.mes-hall↗

arXiv2026

Coherent vibrational wave packet motion in ErCry4a proteins monitors the redox state of the flavin chromophore

Cryptochromes are blue-light-sensitive flavoproteins that play central roles in biological function. In European robin (Erithacus rubecula) ErCry4a proteins, optical excitation of their flavin chromophore forms a long-lived radical pair through a sequence of electron transfer steps across a tetradic chain of tryptophan residues, making them primary candidates for magnetoreception in night migratory songbirds. Recent quantum chemical calculations indicate that nonadiabatic couplings play a central role in the energy and charge transfer processes initiated by optical excitation. Here, we study these dynamics in ErCry4a using ultrafast transient absorption spectroscopy with 10-fs time resolution in the 450-nm spectral range. We uncover a rapid, sub-50 fs red shift in stimulated emission, quenched within 360 fs by electron transfer from a nearby tryptophan moiety. While high-frequency excited state vibrations are rapidly damped, coherent motion involving several low-frequency vibrations persists during both the initial energy relaxation and the subsequent electron transfer. This is evidenced by probing the coherent vibrational motion of the formed FAD$^{\bullet-}$ radical anion and is independently validated by blocking the electron transfer through site-selective tryptophan mutation. Our results only provide insight into the role of nonadiabatic couplings for the initial steps of cryptochrome photoactivation and suggest a general strategy for redox-state-specific monitoring of charge transfer dynamics by probing coherent vibrational motion.

physics.chem-ph↗

arXiv2026

Strong coupling regimes of an organic exciton mirror in a microcavity

The coherent, periodic energy transfer between light- and matter excitations characterizes the strong coupling regime of cavity exciton-polaritons, resulting, in the simplest case, in a Rabi-doublet in the spectral domain. We demonstrate a peculiar regime of strong light-matter coupling, which arises when photonic cavity modes couple to an ultra-thin excitonic mirror. We embed a 12 nm J-aggregated thin film in an open microcavity and tune the coupling strength from weak to the onset of ultrastrong coupling. At resonance, the excitonic mirror selectively changes dielectric to metallic field boundary conditions adding a 2π phase, which links optical cavity modes of different order. Our work gives an exciting perspective to ultra-fast cavity switches and photonic devices based on excitonic optical elements.

cond-mat.mes-hall↗

arXiv2026

Nonadiabatic couplings drive ultrafast, mode-selective intramolecular vibrational energy redistribution in flavins

Flavins are the chromophores in several blue-light-sensitive photoreceptor proteins and act as redox cofactors in many enzymes relevant for biological processes. Despite their biological relevance and numerous, detailed optical investigations of their photophysical properties, the ultrafast nonequilibrium dynamics of their elementary optical excitations are not yet fully known. Here, we use ultrafast coherent vibrational spectroscopy with 10-fs time resolution in the 450-nm spectral range to study their excited state coherent vibrational dynamics. We observe that coherent wavepacket motion along high-frequency C-C stretching modes with ~ 20-fs period is rapidly damped on a 20-fs timescale. In contrast, coherent motion along several low-frequency modes persists much longer. We attribute this to a mode-selective intramolecular vibrational energy redistribution driven by nonadiabatic couplings between the optical bright state and a close-lying dark electronic state, in accordance with model calculations. Our results may be of relevance for the formation of long-lived radical pair states in magnetic-field sensitive proteins.

physics.chem-ph↗

arXiv2025

Ultrafast dynamics of coherent exciton-polaritons in van der Waals semiconductor metasurfaces

Enabling coherent light-matter interactions is a critical step toward next-generation quantum technologies. However, achieving this under ambient temperature conditions remains challenging due to rapid dephasing in optically excited systems. Optical metasurfaces based on quasi-bound states in the continuum have recently emerged as a powerful platform for reaching the strong light-matter coupling regime in flat, subwavelength thickness devices. Here, we investigate ultrafast exciton-polariton dynamics in self-hybridized WS$_2$ thin-film metasurfaces. Using hyperspectral momentum-resolved imaging, we reconstruct the highly anisotropic exciton-polariton dispersion, with a transition from positive to negative effective mass along orthogonal symmetry axes. Femtosecond pump-probe and multidimensional spectroscopy reveal detuning-dependent polariton dynamics with a coherence time up to ~110 fs, and allow direct observation of the coherent dynamics through ultrafast Rabi oscillations with ~45 fs period. We describe this behaviour with a three-eigenstate model that couples the photonic resonance with both bright and dark excitons, extending the conventional two-state picture of strong coupling. Our results establish van der Waals metasurfaces as a promising platform for next-generation polaritonic devices, enabling coherent quantum transfer of matter excitations at room temperature.

physics.optics↗

arXiv2025

Ultrafast transition from coherent to incoherent polariton nonlinearities in a hybrid 1L-WS2/plasmon structure

Exciton polaritons based on atomically thin semiconductors are essential building blocks of quantum optoelectronic devices. Their properties are governed by an ultrafast and oscillatory energy transfer between their excitonic and photonic constituents, resulting in the formation of polaritonic quasiparticles with pronounced nonlinearities induced by the excitonic component. In metallic nanoresonators, dissipation phenomena limit the polariton lifetime to a few ten femtoseconds, so short that the role of these polaritons for the nonlinearities of such hybrids is yet unexplored. Here, we use ultrafast two-dimensional electronic spectroscopy (2DES) to uncover coherent polariton dynamics in a hybrid monolayer (1L) WS2/plasmonic nanostructure. With respect to an uncoupled WS2 flake, we observe an over 20-fold, polarization-dependent enhancement of the optical nonlinearity and a rapid evolution of the 2DES spectra within ~70 fs. We relate these dynamics to a transition from coherent polaritons to incoherent excitations, unravel the microscopic optical nonlinearities, and show the potential of coherent polaritons for ultrafast all-optical switching.

cond-mat.mes-hall↗

arXiv2025

Roadmap for Photonics with 2D Materials

Triggered by the development of exfoliation and the identification of a wide range of extraordinary physical properties in self-standing films consisting of one or few atomic layers, two-dimensional (2D) materials such as graphene, transition metal dichalcogenides (TMDs), and other van der Waals (vdW) crystals currently constitute a wide research field protruding in multiple directions in combination with layer stacking and twisting, nanofabrication, surface-science methods, and integration into nanostructured environments. Photonics encompasses a multidisciplinary collection of those directions, where 2D materials contribute with polaritons of unique characteristics such as strong spatial confinement, large optical-field enhancement, long lifetimes, high sensitivity to external stimuli (e.g., electric and magnetic fields, heating, and strain), a broad spectral range from the far infrared to the ultraviolet, and hybridization with spin and momentum textures of electronic band structures. The explosion of photonics with 2D materials as a vibrant research area is producing breakthroughs, including the discovery and design of new materials and metasurfaces with unprecedented properties as well as applications in integrated photonics, light emission, optical sensing, and exciting prospects for applications in quantum information, and nanoscale thermal transport. This Roadmap summarizes the state of the art in the field, identifies challenges and opportunities, and discusses future goals and how to meet them through a wide collection of topical sections prepared by leading practitioners.

cond-mat.mtrl-sci↗

arXiv2024

Two-dimensional electronic spectroscopy of organic semiconductor nanostructures

This chapter discusses recent experimental work exploring the optical properties and quantum dynamics of organic semiconductor nanostructures based on squaraine dyes. Squaraines are prototypical quadrupolar charge-transfer chromophores of interest for solu-tion-processed photovoltaics and as aggregates with large circular dichroism. Here, we demonstrate and exploit their unique properties as quantum emitters for implementing hy-brid nanostructures featuring strong exciton-plasmon couplings. We show that the unusual electronic properties of squaraines result in a substantial reduction of vibronic coupling to the ubiquitous high-frequency C-C-bond-stretching modes of organic materials and in the formation of spectrally narrow J-aggregated exciton resonances in squaraine thin films. This is exploited to create metallic nanostructures covered with squaraine thin films and to per-form the first time-domain study of coherent exciton-plasmon couplings using two-dimensional electronic spectroscopy with 10-fs time resolution. The experiments present unexpected evidence for long-range coherent exciton transport driven by plasmonic fields. This opens up new opportunities for manipulating the coherent transport of matter excita-tions by coupling to vacuum fields.

cond-mat.mtrl-sci↗

arXiv2024

Phase-cycling and double-quantum two-dimensional electronic spectroscopy using a common-path birefringent interferometer

Selecting distinct quantum pathways in two-dimensional electronic spectroscopy (2DES) can give particularly deep insights into coherent and incoherent interactions and quantum dynamics in various materials. This includes isolating rephasing and non-rephasing pathways for conventional single-quantum 2DES, but also the ability to record double- and zero-quantum spectra. Such advanced 2DES schemes usually require phase-cycling when performed in a partially or fully collinear geometry. A particularly simple and effective implementation of 2DES utilizes an in-line birefringent interferometer, the Translating-Wedge-based Identical pulses eNcoding System (TWINS), for the generation of an inherently phase-stable collinear excitation pulse pair. Here, we demonstrate how the TWINS can be adapted to allow for phase-cycling and experimental access to isolated quantum pathways. These new capabilities are demonstrated by recording rephasing, non-rephasing, zero-quantum and double-quantum 2DES on a molecular J-aggregate. This easy-to-implement extension opens up new experimental possibilities for TWINS-based 2DES in multidimensional all-optical and photoemission spectroscopy and microscopy.

physics.chem-ph↗

arXiv2023

Two-dimensional electronic spectroscopy from first principles

The recent development of multidimensional ultrafast spectroscopy techniques calls for the introduction of computational schemes that allow for the simulation of such experiments and the interpretation of the corresponding results from a microscopic point of view. In this work, we present a general and efficient first-principles scheme to compute two-dimensional electronic spectroscopy maps based on real-time time-dependent density-functional theory. The interface of this approach with the Ehrenfest scheme for molecular dynamics enables the inclusion of vibronic effects in the calculations based on a classical treatment of the nuclei. The computational complexity of the simulations is reduced by the application of numerical advances such as branching techniques, undersampling, and a novel reduced phase cycling scheme, applicable for systems with inversion symmetry. We demonstrate the effectiveness of this method by applying it to prototypical molecules such as benzene, pyridine, and pyrene. We discuss the role of the approximations that inevitably enter the adopted theoretical framework and set the stage for further extensions of the proposed method to more realistic systems.

cond-mat.mes-hall↗

arXiv2023

Plasmon mediated coherent population oscillations in molecular aggregates

The strong coherent coupling of quantum emitters to vacuum fluctuations of the light field offers opportunities for manipulating the optical and transport properties of nanomaterials, with potential applications ranging from ultrasensitive all-optical switching to creating polariton condensates. Often, ubiquitous decoherence processes at ambient conditions limit these couplings to such short time scales that the quantum dynamics of the interacting system remains elusive. Prominent examples are strongly coupled exciton-plasmon systems, which, so far, have mostly been investigated by linear optical spectroscopy. Here, we use ultrafast two-dimensional electronic spectroscopy to probe the quantum dynamics of J-aggregate excitons collectively coupled to the spatially structured plasmonic fields of a gold nanoslit array. We observe rich coherent Rabi oscillation dynamics reflecting a plasmon-driven coherent exciton population transfer over mesoscopic distances at room temperature. This opens up new opportunities to manipulate the coherent transport of matter excitations by coupling to vacuum fields.

cond-mat.mes-hall↗

arXiv2023

Ultra-bright single photon source based on an atomically thin material

Solid-state single photon sources are central building blocks in quantum communication networks and on-chip quantum information processing. Atomically thin crystals were established as possible candidates to emit non-classical states of light, however, the performance of monolayer-based single photon sources has so far been lacking behind state-of-the-art devices based on volume crystals. Here, we implement a single photon source based on an atomically thin sheet of WSe2 coupled to a spectrally tunable optical cavity. It is characterized by a high single photon purity with a $g^{(2)}(0)$ value as low as $4.7 \pm 0.7 \%$ and a record-high first lens brightness of linearly polarized photons as large as $65 \pm 4 \%$. Interestingly, the high performance of our devices allows us to observe genuine quantum interference phenomena in a Hong-Ou-Mandel experiment. Our results demonstrate that open cavities and two-dimensional materials constitute an excellent platform for ultra-bright quantum light sources: the unique properties of such two-dimensional materials and the versatility of open cavities open an inspiring avenue for novel quantum optoelectronic devices.

quant-ph↗

arXiv2022

Tracking the Electron Transfer Cascade in European Robin Cryptochrome 4 Mutants

The primary step in the elusive ability of migratory birds to sense weak Earth-strength magnetic fields is supposedly the light-induced formation of a long-lived, magnetically sensitive radical pair inside a cryptochrome flavoprotein located in the retina of these birds. Blue light absorption by a flavin chromophore triggers a series of sequential electron transfer steps across a tetradic tryptophan chain towards the flavin acceptor. The recent ability to express cryptochrome 4 from the night-migratory European robin (Erithacus rubecula), ErCry4, and to replace the tryptophan residues individually by a redox-inactive phenylalanine offers the prospect of exploring the role of each of the tryptophan residues in the electron transfer chain. Here, we compare ultrafast transient absorption spectroscopy of wild type ErCry4 and four of its mutants having phenylalanine residues in different positions of the chain. In the mutants we observe that each of the first three tryptophan residues in the chain adds a distinct relaxation component (time constants 0.5, 30 and 150 ps) to the transient absorption data. The dynamics in the mutant with a terminal phenylalanine residue are very similar to those in wild type ErCry4, excepted for a reduced concentration of long-lived radical pairs. The experimental results are evaluated and discussed in connection with Marcus-Hopfield theory, providing a complete microscopic insight into the sequential electron transfers across the tryptophan chain. Our results offer a path to studying spin transport and dynamical spin correlations in flavoprotein radical pairs.

physics.chem-ph↗

arXiv2021

Strong inelastic scattering of slow electrons by optical near fields of small nanoparticles

The interaction of swift, free-space electrons with confined optical near fields has recently sparked much interest. It enables a new type of photon-induced near-field electron microscopy, mapping local optical near fields around nanoparticles with exquisite spatial and spectral resolution and lies at the heart of quantum state manipulation and attosecond pulse shaping of free electrons. The corresponding interaction of optical near fields with slow electrons has achieved much less attention, even though the lower electron velocity may enhance electron-near-field coupling for small nanoparticles. A first-principle theoretical study of such interactions has been reported very recently [N. Talebi, Phys. Rev. Lett. 125, 080401 (2020)]. Building up on this work, we investigate, both analytically and numerically, the inelastic scattering of slow electrons by near fields of small nanostructures. For weak fields, this results in distinct angular diffraction patterns that represent, to first order, the Fourier transform of the transverse variation of the scalar near-field potential along the direction perpendicular to the electron propagation. For stronger fields, scattering by the near-field component along the electron trajectory results in a break-up of the energy spectrum into multiple photon orders. Their angular diffraction patterns are given by integer powers of the Fourier transform of the transverse potential variation and are shifting in phase with photon order. Our analytical model offers an efficient approach for studying the effects of electron kinetic energy, near field shape and strength on the diffraction and thus may facilitate the experimental observation of these phenomena by, e.g., ultrafast low-energy point-projection microscopy or related techniques. This could provide simultaneous access to different vectorial components of the optical near fields of small nanoparticles.

quant-ph↗

arXiv2021

Femtosecond field-driven on-chip unidirectional electronic currents in nonadiabatic tunnelling regime

Recently, asymmetric plasmonic nanojunctions [Karnetzky et. al., Nature Comm. 2471, 9 (2018)] have shown promise as on-chip electronic devices to convert femtosecond optical pulses to current bursts, with a bandwidth of multi-terahertz scale, although yet at low temperatures and pressures. Such nanoscale devices are of great interest for novel ultrafast electronics and opto-electronic applications. Here, we operate the device in air and at room temperature, revealing the mechanisms of photoemission from plasmonic nanojunctions, and the fundamental limitations on the speed of optical-to-electronic conversion. Inter-cycle interference of coherent electronic wavepackets results in a complex energy electron distribution and birth of multiphoton effects. This energy structure, as well as reshaping of the wavepackets during their propagation from one tip to the other, determine the ultrafast dynamics of the current. We show that, up to some level of approximation, the electron flight time is well-determined by the mean ponderomotive velocity in the driving field.

cond-mat.mes-hall↗

arXiv2019

Interference between Quantum Paths in Coherent Kapitza-Dirac Effect

In the Kapitza-Dirac effect, atoms, molecules, or swift electrons are diffracted off a standing wave grating of the light intensity created by two counter-propagating laser fields. In ultrafast electron optics, such a coherent beam splitter offers interesting perspectives for ultrafast beam shaping. Here, we study, both analytically and numerically, the effect of the inclination angle between two laser fields on the diffraction of pulsed, low-energy electron beams. For sufficiently high light intensities, we observe a rich variety of complex diffraction patterns. These do not only reflect interferences between electrons scattered off intensity gratings that are formed by different vector components of the laser field. They may also result, for certain light intensities and electron velocities, from interferences between these ponderomotive scattering and direct light absorption and stimulated emission processes, usually forbidden for far-field light. Our findings may open up perspectives for the coherent manipulation and control of ultrafast electron beams by free-space light.

quant-ph↗

arXiv2019

Bridging Microscopic Nonlinear Polarizations toward Far-Field Second Harmonic Radiation

Since the first observation of second harmonic generation (SHG), there have been extensive studies on this nonlinear phenomenon not only to clarify its physical origin but also to realize unconventional functionalities. Nonetheless, a widely accepted model of SHG with rigorous experimental verification that describes the contributions of different underlying microscopic mechanisms is still under debate. Here, we examine second harmonic far-field radiation patterns over a wide angle from metallic structures with different resonances, to reveal the structure-dependent contributions from distinct nonlinear polarizations. By comparing the measured SHG radiation patterns of 82 antennas with different SHG models, we demonstrate the critical role of the surface-parallel and bulk nonlinear polarizations in the far-field SHG patterns, and thus show that the common belief of the dominant contribution of the surface-normal component in SHG should be corrected. A virtual multi-resonator SHG model inside a single physical resonator is introduced to explain and control the interplay between different nonlinear polarizations and their structure-dependent excitations. Our findings offer a new strategy for the design of highly efficient and directional nonlinear metamaterials.

physics.optics↗

arXiv2018

Strong spatial and spectral localization of surface plasmons in individual randomly disordered gold nanosponges

Porous nanosponges, percolated with a three-dimensional network of 10-nm sized ligaments, recently emerged as promising substrates for plasmon-enhanced spectroscopy and (photo-)catalysis. Experimental and theoretical work suggests surface plasmon localization in some hot-spot modes as the physical origin of their unusual optical properties, but so far the existence of such hot-spots has not been proven. Here we use scattering-type scanning near-field nano-spectroscopy on individual gold nanosponges to reveal spatially and spectrally confined modes with 10 nanometer localization lengths by mapping the local optical density of states. High quality factors of individual hot-spots of more than 40 are demonstrated. A statistical analysis of near-field intensity fluctuations unveils plasmonics in the strong localization regime. The observed field localization and enhancement make such nanosponges an appealing platform for a variety of applications ranging from nonlinear optics to strong-coupling physics.

cond-mat.mes-hall↗