arXiv subjects

Hélène Seiler

Publications and source records attributed to Hélène Seiler.

13 recordsLinked to original sources

arXiv2026

Coherent two-dimensional electronic spectroscopy integrated with confocal back focal plane microscopy

We introduce a setup for coherent two-dimensional electronic spectroscopy in the pump-probe reflection geometry that is integrated with a confocal back focal plane imaging microscope. The angle-resolved capability is utilized to control pump and probe wavevectors, while real space imaging enables co-localization of the collection spots for linear and ultrafast experiments. Compression of pulses down to 20 fs is achieved. We demonstrate the capabilities of this approach on an exfoliated WSe$_2$ monolayer on Si/SiO$_2$. The setup is suited to investigate excitons and exciton-polaritons in 2D Materials and their heterostructures.

cond-mat.mtrl-sci↗

arXiv2025

Directed light emission from monolayers on 2D materials via optical interferences

Two-dimensional materials provide a rich platform to explore phenomena such as emerging electronic and excitonic states, strong light-matter coupling and new optoelectronic device concepts. The optical response of monolayers is entangled with the substrate on which they are grown or deposited on, often a two-dimensional material itself. Understanding how the properties of the two-dimensional monolayers can be tuned via the substrate is therefore essential. Here we employ angle-resolved reflectivity and photoluminescence spectroscopy on highly ordered molecular monolayers on hexagonal boron nitride (hBN) to systematically investigate the angle-dependent optical response as a function of the thickness of the hBN flake. We observe that light reflection and emission occur in a strongly directed fashion and that the direction of light reflection and emission is dictated by the hBN flake thickness. Transfer matrix simulations reproduce the experimental data and show that optical interference effects in hBN are at the origin of the angle-dependent optical properties. While our study focuses on molecular monolayers on hBN, our findings are general and relevant for any 2D material placed on top of a substrate. Our findings demonstrate the need to carefully choose substrate parameters for a given experimental geometry but also highlight opportunities in applications such as lighting technology where the direction of light emission can be controlled via substrate thickness.

cond-mat.mes-hall↗

arXiv2025

Momentum-Resolved Signatures of Carrier Screening Effects on Electron-Phonon Coupling in MoS$_2$

Electron-phonon coupling is central to many condensed matter phenomena. Harnessing these effects for novel material functionality in materials always involves non-equilibrium electronic states, which in turn alter quasi-free-carrier density and screening. Thus, gaining a fundamental understanding of the interplay of carrier screening and electron-phonon coupling is essential for advancing ultrafast science. Prior works have mainly focused on the impact of carrier screening on electronic structure properties. Here we investigate the non-equilibrium lattice dynamics of MoS2 after a photoinduced Mott transition. The experimental data are closely reproduced by ab-initio ultrafast dynamics simulations. We find that the non-thermal diffuse scattering signals in the vicinity of the Bragg peaks, originating from long-wavelength phonon emission, can only be reproduced upon explicitly accounting for the screening of electron-phonon interaction introduced by the Mott transition. These results indicate the screening influences electron-phonon coupling, leading to a suppression of intravalley phonon-assisted carrier relaxation. Overall, the combined experimental and computational approach introduced here offers new prospects for exploring the influence of screening of the electron-phonon interactions and relaxation pathways in driven solids.

cond-mat.mtrl-sci↗

arXiv2022

Observation of multi-directional energy transfer in a hybrid plasmonic-excitonic nanostructure

Hybrid plasmonic devices involve a nanostructured metal supporting localized surface plasmons to amplify light-matter interaction, and a non-plasmonic material to functionalize charge excitations. Application-relevant epitaxial heterostructures, however, give rise to ballistic ultrafast dynamics that challenge the conventional semiclassical understanding of unidirectional nanometal-to-substrate energy transfer. We study epitaxial Au nanoislands on WSe$_2$ with time- and angle-resolved photoemission spectroscopy and femtosecond electron diffraction: this combination of techniques resolves material, energy and momentum of charge-carriers and phonons excited in the heterostructure. We observe a strong non-linear plasmon-exciton interaction that transfers the energy of sub-bandgap photons very efficiently to the semiconductor, leaving the metal cold until non-radiative exciton recombination heats the nanoparticles on hundreds of femtoseconds timescales. Our results resolve a multi-directional energy exchange on timescales shorter than the electronic thermalization of the nanometal. Electron-phonon coupling and diffusive charge-transfer determine the subsequent energy flow. This complex dynamics opens perspectives for optoelectronic and photocatalytic applications, while providing a constraining experimental testbed for state-of-the-art modelling.

cond-mat.mes-hall↗

arXiv2022

Direct observation of ultrafast lattice distortions during exciton-polaron formation in lead-halide perovskite nanocrystals

The microscopic origin of slow carrier cooling in lead-halide perovskites remains debated, and has direct implications for applications. Slow carrier cooling has been attributed to either polaron formation or a hot-phonon bottleneck effect at high excited carrier densities (> 10$^{18}$ cm$^{-3}$). These effects cannot be unambiguously disentangled from optical experiments alone. However, they can be distinguished by direct observations of ultrafast lattice dynamics, as these effects are expected to create qualitatively distinct fingerprints. To this end, we employ femtosecond electron diffraction and directly measure the sub-picosecond lattice dynamics of weakly confined CsPbBr$_3$ nanocrystals following above-gap photo-excitation. The data reveal a light-induced structural distortion appearing on a time scale varying between 380 fs to 1200 fs depending on the excitation fluence. We attribute these dynamics to the effect of exciton-polarons on the lattice, and the slower dynamics at high fluences to slower hot carrier cooling, which slows down the establishment of the exciton-polaron population. Further analysis and simulations show that the distortion is consistent with motions of the [PbBr$_3$]$^{-}$ octahedral ionic cage, and closest agreement with the data is obtained for Pb-Br bond lengthening. Our work demonstrates how direct studies of lattice dynamics on the sub-picosecond timescale can discriminate between competing scenarios, thereby shedding light on the origin of slow carrier cooling in lead-halide perovskites.

cond-mat.mtrl-sci↗

arXiv2022

Intrinsic energy flow in laser-excited 3$d$ ferromagnets

Ultrafast magnetization dynamics are governed by energy flow between electronic, magnetic, and lattice degrees of freedom. A quantitative understanding of these dynamics must be based on a model that agrees with experimental results for all three subsystems. However, ultrafast dynamics of the lattice remain largely unexplored experimentally. Here, we combine femtosecond electron diffraction experiments of the lattice dynamics with energy-conserving atomistic spin dynamics (ASD) simulations and ab-initio calculations to study the intrinsic energy flow in the 3d ferromagnets cobalt (Co) and iron (Fe). The simulations yield a good description of experimental data, in particular an excellent description of our experimental results for the lattice dynamics. We find that the lattice dynamics are influenced significantly by the magnetization dynamics due to the energy cost of demagnetization. Our results highlight the role of the spin system as the dominant heat sink in the first hundreds of femtoseconds. Together with previous findings for nickel [Zahn et al., Phys. Rev. Research 3, 023032 (2021)], our work demonstrates that energy-conserving ASD simulations provide a general and consistent description of the laser-induced dynamics in all three elemental 3d ferromagnets.

cond-mat.mtrl-sci↗

arXiv2021

Ultrafast lattice dynamics and electron-phonon coupling in platinum extracted with a global fitting approach for time-resolved polycrystalline diffraction data

Quantitative knowledge of electron-phonon coupling is important for many applications as well as for the fundamental understanding of nonequilibrium relaxation processes. Time-resolved diffraction provides direct access to this knowledge through its sensitivity to laser-induced lattice dynamics. Here, we present an approach for analyzing time-resolved polycrystalline diffraction data. A two-step routine is used to minimize the number of time-dependent fit parameters. The lattice dynamics are extracted by finding the best fit to the full transient diffraction pattern rather than by analyzing transient changes of individual Debye-Scherrer rings. We apply this approach to platinum, an important component of novel photocatalytic and spintronic applications, for which a large variation of literature values exists for the electron-phonon coupling parameter $G_\mathrm{ep}$. Based on the extracted evolution of the atomic mean squared displacement (MSD) and using a two-temperature model (TTM), we obtain $G_\mathrm{ep}=(3.9\pm0.2)\cdot10^{17}\frac{\mathrm{W}}{\mathrm{m}^3\hspace{1pt}\mathrm{K}}$ (statistical error). We find that at least up to an absorbed energy density of $124\hspace{2pt}\frac{\mathrm{J}}{\mathrm{cm}^3}$, $G_\mathrm{ep}$ is not fluence-dependent. Our results for the lattice dynamics of platinum provide insights into electron-phonon coupling and phonon thermalization and constitute a basis for quantitative descriptions of platinum-based heterostructures in nonequilibrium conditions.

cond-mat.mtrl-sci↗

arXiv2021

Multi-phonon diffuse scattering in solids from first-principles: Application to layered crystals and 2D materials

Time-resolved diffuse scattering experiments have gained increasing attention due to their potential to reveal non-equilibrium dynamics of crystal lattice vibrations with full momentum resolution. Although progress has been made in interpreting experimental data on the basis of one-phonon scattering, understanding the role of individual phonons can be sometimes hindered by multi-phonon excitations. In Ref. [{\it arXiv:2103.10108}] we have introduced a rigorous approach for the calculation of the all-phonon inelastic scattering intensity of solids from first-principles. In the present work, we describe our implementation in detail and show that multi-phonon interactions are captured efficiently by exploiting translational and time-reversal symmetries of the crystal. We demonstrate its predictive power by calculating the scattering patterns of monolayer molybdenum disulfide (MoS$_2$), bulk MoS$_2$, and black phosphorus (bP), and we obtain excellent agreement with our measurements of thermal electron diffuse scattering. Remarkably, our results show that multi-phonon excitations dominate in bP across multiple Brillouin zones, while in MoS$_2$ they play a less pronounced role. We expand our analysis for each system and examine the effect of individual atomic and interatomic vibrational motion on the diffuse scattering signals. We further demonstrate the high-throughput capability of our approach by reporting all-phonon scattering maps of 2D MoSe2, WSe2, WS2, graphene, and CdI2, rationalizing in each case the effect of multi-phonon processes. As a side point, we show that the special displacement method reproduces the thermally distorted configuration that generates precisely the all-phonon diffuse pattern.

cond-mat.mtrl-sci↗

arXiv2021

Efficient first-principles methodology for the calculation of the all-phonon inelastic scattering in solids

Inelastic scattering experiments are key methods for mapping the full dispersion of fundamental excitations of solids in the ground as well as non-equilibrium states. A quantitative analysis of inelastic scattering in terms of phonon excitations requires identifying the role of multi-phonon processes. Here, we develop an efficient first-principles methodology for calculating the all-phonon quantum mechanical structure factor of solids. We demonstrate our method by obtaining excellent agreement between measurements and calculations of the diffuse scattering patterns of black phosphorus, showing that multi-phonon processes play a substantial role. The present approach constitutes a step towards the interpretation of static and time-resolved electron, X-ray, and neutron inelastic scattering data.

cond-mat.mtrl-sci↗

arXiv2021

Accessing the anisotropic non-thermal phonon populations in black phosphorus

We combine femtosecond electron diffuse scattering experiments and first-principles calculations of the coupled electron-phonon dynamics to provide a detailed momentum-resolved picture of the ultrafast lattice thermalization in a thin film of black phosphorus. The measurements reveal the emergence of highly anisotropic non-thermal phonon populations which persist for several picoseconds following excitation of the electrons with a light pulse. Combining ultrafast dynamics simulations based on the time-dependent Boltzmann formalism and calculations of the structure factor, we reproduce the experimental data and identify the vibrational modes primarily responsible for the carrier relaxation via electron-phonon coupling and the subsequent lattice thermalization via phonon-phonon scattering. In particular, we attribute the non-equilibrium lattice dynamics of black phosphorus to highly-anisotropic phonon-assisted scattering processes, which are primarily mediated by high-energy optical phonons. Our approach paves the way towards unravelling and controlling microscopic energy-flow pathways in two-dimensional materials and van der Waals heterostructures, and may also be extended to other non-equilibrium phenomena involving coupled electron-phonon dynamics such as superconductivity, phase transitions or polaron physics.

cond-mat.mes-hall↗

arXiv2021

Lattice dynamics and ultrafast energy flow between electrons, spins, and phonons in a 3d ferromagnet

The ultrafast dynamics of magnetic order in a ferromagnet are governed by the interplay between electronic, magnetic and lattice degrees of freedom. In order to obtain a microscopic understanding of ultrafast demagnetization, information on the response of all three subsystems is required. A consistent description of demagnetization and microscopic energy flow, however, is still missing. Here, we combine a femtosecond electron diffraction study of the ultrafast lattice response of nickel to laser excitation with ab initio calculations of the electron-phonon interaction and energy-conserving atomistic spin dynamics simulations. Our model is in agreement with the observed lattice dynamics and previously reported electron and magnetization dynamics. Our approach reveals that the spin system is the dominating heat sink in the initial few hundreds of femtoseconds and implies a transient non-thermal state of the spins. Our results provide a clear picture of the microscopic energy flow between electronic, magnetic and lattice degrees of freedom on ultrafast timescales and constitute a foundation for theoretical descriptions of demagnetization that are consistent with the dynamics of all three subsystems.

cond-mat.mtrl-sci↗

arXiv2020

Nuclear dynamics of singlet exciton fission: a direct observation in pentacene single crystals

Singlet exciton fission (SEF) is a key process in the development of efficient opto-electronic devices. An aspect that is rarely probed directly, and yet has a tremendous impact on SEF properties, is the nuclear structure and dynamics involved in this process. Here we directly observe the nuclear dynamics accompanying the SEF process in single crystal pentacene using femtosecond electron diffraction. The data reveal coherent atomic motions at 1 THz, incoherent motions, and an anisotropic lattice distortion representing the polaronic character of the triplet excitons. Combining molecular dynamics simulations, time-dependent density functional theory and experimental structure factor analysis, the coherent motions are identified as collective sliding motions of the pentacene molecules along their long axis. Such motions modify the excitonic coupling between adjacent molecules. Our findings reveal that long-range motions play a decisive part in the disintegration of the electronically correlated triplet pairs, and shed light on why SEF occurs on ultrafast timescales.

physics.chem-ph↗

arXiv2020

Anisotropic Nonequilibrium Lattice Dynamics of Black Phosphorus

Black phosphorus has recently attracted significant attention for its highly anisotropic properties. A variety of ultrafast optical spectroscopies has been applied to probe the carrier response to photoexcitation, but the complementary lattice response has remained unaddressed. Here we employ femtosecond electron diffraction to explore how the structural anisotropy impacts the lattice dynamics after photoexcitation. We observe two timescales in the lattice response, which we attribute to electron-phonon and phonon-phonon thermalization. Pronounced differences between armchair and zigzag directions are observed, indicating a nonthermal state of the lattice lasting up to ~60 ps. This nonthermal state is characterized by a modified anisotropy of the atomic vibrations compared to equilibrium. Our findings provide insights in both electron-phonon as well as phonon-phonon coupling and bear direct relevance for any application of black phosphorus in nonequilibrium conditions.

cond-mat.mtrl-sci↗