arXiv subjects

Jonas Zipfel

Publications and source records attributed to Jonas Zipfel.

18 recordsLinked to original sources

arXiv2023

Phason-mediated interlayer exciton diffusion in WS2/WSe2 moir\'e heterostructure

Moir\'e potentials in two-dimensional materials have been proven to be of fundamental importance to fully understand the electronic structure of van der Waals heterostructures, from superconductivity to correlated excitonic states. However, understanding how the moir\'e phonons, so-called phasons, affect the properties of the system still remains an uncharted territory. In this work, we demonstrate how phasons are integral to properly describing and understanding low-temperature interlayer exciton diffusion in WS2/WSe2 heterostructure. We perform photoluminescence (PL) spectroscopy to understand how the coupling between the layers, affected by their relative orientation, impacts the excitonic properties of the system. Samples fabricated with stacking angles of 0{\deg} and 60{\deg} are investigated taking into account the stacking angle dependence of the two common moir\'e potential profiles. Additionally, we present spatially and time-resolved exciton diffusion measurements, looking at the photoluminescence emission in a temperature range from 30 K to 250 K. An accurate potential for the two configurations are computed via density functional theory (DFT) calculations. Finally, we perform molecular dynamics simulation in order to visualize the phasons motion, estimating the phason speed at different temperatures, providing novel insights into the mechanics of exciton propagation at low temperatures that cannot be explained within the frame of classical exciton diffusion alone.

cond-mat.mtrl-sci↗

arXiv2022

Hyperspectral imaging of excitons within a moir\'e unit-cell with a sub-nanometer electron probe

Electronic and optical excitations in two-dimensional moir\'e systems are uniquely sensitive to local atomic registries, leading to materials- and twist-angle specific correlated electronic ground states with varied degree of localization. However, there has been no direct experimental correlation between the sub-nanometer structure and emergent excitonic transitions, comprising tightly-bound pairs of photoexcited electrons and holes. Here, we use cryogenic transmission electron microscopy and spectroscopy to simultaneously image the structural reconstruction and associated localization of the lowest-energy intralayer exciton in a rotationally aligned heterostructure of WS2 and WSe2 monolayers. In conjunction with optical spectroscopy and ab initio calculations, we determine that the exciton center-of-mass wavefunction is strongly modulated in space, confined to a radius of ~ 2 nm around the highest-energy stacking site in the moir\'e unit-cell, forming a triangular lattice. Our results provide direct evidence that atomic reconstructions lead to the strongly confining moir\'e potentials and that engineering strain at the nanoscale will enable new types of excitonic lattices.

cond-mat.mtrl-sci↗

arXiv2021

Electron recoil effect in electrically tunable MoSe2 monolayers

Radiative recombination of excitons dressed by the interactions with free charge carriers often occurs under simultaneous excitation of either electrons or holes to unbound states. This phenomenon, known as the electron recoil effect, manifests itself in pronounced, asymmetric spectral lineshapes of the resulting emission. We study the electron recoil effect experimentally in electrically-tunable monolayer semiconductors and derive it theoretically using both trion and Fermi-polaron pictures. Time-resolved analysis of the recoil lineshapes is employed to access transient, non-equilibrium states of the exciton-carrier complexes. We demonstrate cooling of the initially overheated populations on the picosecond timescales and reveal the impact of lattice temperature and free carrier density. Both thermally activated phonons and the presence of free charges are shown to accelerate equilibration. Finally, we find strong correlations between relaxation times from recoil analysis and luminescence rise times, providing a consistent interpretation for the initial dynamics of trion/Fermi-polaron states.

cond-mat.mes-hall↗

arXiv2021

Interlayer exciton valley polarization dynamics in large magnetic fields

In van der Waals heterostructures (HS) consisting of stacked MoSe$_2$ and WSe$_2$ monolayers, optically bright interlayer excitons (ILE) can be observed when the constituent layers are crystallographically aligned. The symmetry of the monolayers allows for two different types of alignment, in which the momentum-direct interlayer transitions are either valley-conserving (R-type alignment) or changing the valley index (H-type anti-alignment). Here, we study the valley polarization dynamics of ILE in magnetic fields up to 30~Tesla by time-resolved photoluminescence (PL). For all ILE types, we find a finite initial PL circular degree of polarization ($DoP$) after unpolarized excitation in applied magnetic fields. For ILE in H-type HS, we observe a systematic increase of the PL $DoP$ with time in applied magnetic fields, which saturates at values close to unity for the largest fields. By contrast, for ILE in R-type HS, the PL $DoP$ shows a decrease and a zero crossing before saturating with opposite polarization. This unintuitive behavior can be explained by a model considering the different ILE states in H- and R-type HS and their selection rules coupling PL helicity and valley polarization.

cond-mat.mes-hall↗

arXiv2021

Nonclassical Exciton Diffusion in Monolayer WSe2

We experimentally demonstrate time-resolved exciton propagation in a monolayer semiconductor at cryogenic temperatures. Monitoring phonon-assisted recombination of dark states, we find a highly unusual case of exciton diffusion. While at 5 K the diffusivity is intrinsically limited by acoustic phonon scattering, we observe a pronounced decrease of the diffusion coefficient with increasing temperature, far below the activation threshold of higher-energy phonon modes. This behavior corresponds neither to well-known regimes of semiclassical free-particle transport nor to the thermally activated hopping in systems with strong localization. Its origin is discussed in the framework of both microscopic numerical and semi-phenomenological analytical models illustrating the observed characteristics of nonclassical propagation. Challenging the established description of mobile excitons in monolayer semiconductors, these results open up avenues to study quantum transport phenomena for excitonic quasiparticles in atomically-thin van der Waals materials and their heterostructures.

cond-mat.mes-hall↗

arXiv2021

Non-equilibrium diffusion of dark excitons in atomically thin semiconductors

Atomically thin semiconductors provide an excellent platform to study intriguing many-particle physics of tightly-bound excitons. In particular, the properties of tungsten-based transition metal dichalcogenides are determined by a complex manifold of bright and dark exciton states. While dark excitons are known to dominate the relaxation dynamics and low-temperature photoluminescence, their impact on the spatial propagation of excitons has remained elusive. In our joint theory-experiment study, we address this intriguing regime of dark state transport by resolving the spatio-temporal exciton dynamics in hBN-encapsulated WSe$_2$ monolayers after resonant excitation. We find clear evidence of an unconventional, time-dependent diffusion during the first tens of picoseconds, exhibiting strong deviation from the steady-state propagation. Dark exciton states are initially populated by phonon emission from the bright states, resulting in creation of hot excitons whose rapid expansion leads to a transient increase of the diffusion coefficient by more than one order of magnitude. These findings are relevant for both fundamental understanding of the spatio-temporal exciton dynamics in atomically thin materials as well as their technological application by enabling rapid diffusion.

cond-mat.mes-hall↗

arXiv2020

Complete polarization of electronic spins in OLEDs

At low temperatures and high magnetic fields, electron and hole spins in an organic light-emitting diode (OLED) become polarized so that recombination preferentially forms molecular triplet excited-state species. For low device currents, magnetoelectroluminescence (MEL) perfectly follows Boltzmann activation, implying a virtually complete polarization outcome. As the current increases, the MEL effect is reduced because spin polarization is suppressed by the reduction in carrier residence time within the device. Under these conditions, an additional field-dependent process affecting the spin-dependent recombination emerges, which appears to relate to the build-up of triplet excitons and the interaction with free charge carriers. Suppression of the EL at high fields on its own does not, strictly, prove electronic spin polarization. We therefore probe changes in the spin statistics of recombination directly in a dual singlettriplet emitting OLED, which shows a concomitant rise in phosphorescence intensity as fluorescence is suppressed. Finite spin-orbit coupling in these materials gives rise to a microscopic distribution in effective g factors of electrons and holes, $Δg$, i.e. a distribution in Larmor frequencies, leading to singlet-triplet mixing within the electronhole pair as a function of applied field. This $Δg$ effect in the pair further suppresses singlet-exciton formation in addition to thermal spin polarization of the individual carriers. Since the $Δg$ process involves weakly bound carrier pairs rather than free electrons and holes, in contrast to thermal spin polarization, the effect does not depend significantly on current or temperature.

cond-mat.mes-hall↗

arXiv2020

Autoionization and dressing of excited excitons by free carriers in monolayer WSe2

We experimentally demonstrate dressing of the excited exciton states by a continuously tunable Fermi sea of free charge carriers in a monolayer semiconductor. It represents an unusual scenario of two-particle excitations of charged excitons previously inaccessible in conventional material systems. We identify excited state trions, accurately determine their binding energies in the zero-density limit for both electron- and hole-doped regimes, and observe emerging many-body phenomena at elevated doping. Combining experiment and theory we gain access to the intra-exciton coupling facilitated by the interaction with free charge carriers. We provide evidence for a process of autoionization for quasiparticles, a unique scattering pathway available for excited states in atomic systems. Finally, we demonstrate a complete transfer of the optical transition strength from the excited excitons to dressed excitons, Fermi polarons, as well as the associated light emission from their non-equilibrium populations.

cond-mat.mes-hall↗

arXiv2020

Fast and anomalous exciton diffusion in two-dimensional hybrid perovskites

Two-dimensional hybrid perovskites are currently in the spotlight of condensed matter and nanotechnology research due to their intriguing optoelectronic and vibrational properties with emerging potential for light-harvesting and -emitting applications. While it is known that these natural quantum wells host tightly bound excitons, the mobilities of these fundamental optical excitations at the heart of the optoelectronic applications are still largely unexplored. Here, we directly monitor the diffusion of excitons through ultrafast emission microscopy from liquid helium to room temperature in hBN-encapsulated two-dimensional hybrid perovskites. We find very fast diffusion with characteristic hallmarks of free exciton propagation for all temperatures above 50 K. In the cryogenic regime we observe nonlinear, anomalous behavior with an exceptionally rapid expansion of the exciton cloud followed by a very slow and even negative effective diffusion. We discuss our findings in view of efficient exciton-phonon coupling, highlighting two-dimensional hybrids as promising platforms for many-body physics research and optoelectronic applications on the nanoscale.

cond-mat.mes-hall↗

arXiv2020

Bright excitons with negative-mass electrons

Bound electron-hole excitonic states are generally not expected to form with charges of negative effective mass. We identify such excitons in a single layer of the semiconductor WSe2, where they give rise to narrow-band upconverted photoluminescence in the UV, at an energy of 1.66 eV above the first band-edge excitonic transition. Negative band curvature and strong electron-phonon coupling result in a cascaded phonon progression with equidistant peaks in the photoluminescence spectrum, resolvable to ninth order. Ab initio GW-BSE calculations with full electron-hole correlations unmask and explain the admixture of upper conduction-band states to this complex many-body excitation: an optically bright, bound exciton in resonance with the semiconductor continuum. This exciton is responsible for atomic-like quantum-interference phenomena such as electromagnetically induced transparency. Since band curvature can be tuned by pressure or strain, synthesis of exotic quasiparticles such as flat-band excitons with infinite reduced mass becomes feasible.

cond-mat.mes-hall↗

arXiv2020

Temporal evolution of low-temperature phonon sidebands in WSe$_2$ monolayers

Low-temperature photoluminescence (PL) of hBN-encapsulated monolayer tungsten diselenide (WSe$_2$) shows a multitude of sharp emission peaks below the bright exciton. Some of them have been recently identified as phonon sidebands of momentum-dark states. However, the exciton dynamics behind the emergence of these sidebands has not been revealed yet. In this joint theory-experiment study, we theoretically predict and experimentally observe time-resolved PL providing microscopic insights into thermalization of hot excitons formed after optical excitation. In good agreement between theory and experiment, we demonstrate a spectral red-shift of phonon sidebands on a timescale of tens of picoseconds reflecting the phonon-driven thermalization of hot excitons in momentum-dark states. Furthermore, we predict the emergence of a transient phonon sideband that vanishes in the stationary PL. The obtained microscopic insights are applicable to a broad class of 2D materials with multiple exciton valleys.

cond-mat.mes-hall↗

arXiv2020

Light-matter coupling and non-equilibrium dynamics of exchange-split trions in monolayer WS2

Monolayers of transition metal dichalcogenides present an intriguing platform to investigate the interplay of excitonic complexes in two dimensional semiconductors. Here, we use optical spectroscopy to study light-matter coupling and non-equilibrium relaxation dynamics of three-particle exciton states, commonly known as trions. We identify the consequences of the exchange interaction for the trion finestructure in tungsten-based monolayer materials from variational calculations and experimentally determine the resulting characteristic differences in their oscillator strength. It allows us to quantitatively extract trion populations from time-resolved photoluminescence measurements and monitor their dynamics after off-resonant optical injection. At liquid helium temperature we observe pronounced non-equilibrium distribution of the trions during their lifetime with comparatively slow equilibration that occurs on time-scales up to several 100's of ps. In addition, we find an intriguing regime of population inversion at lowest excitation densities that builds up and is maintained during 10's of picoseconds. With increased lattice temperature the equilibrium is established more rapidly and the inversion disappears, highlighting the role of thermal activation for efficient scattering between exchange-split trions.

cond-mat.mes-hall↗

arXiv2020

Exciton diffusion in monolayer semiconductors with suppressed disorder

Tightly bound excitons in monolayer semiconductors represent a versatile platform to study two-dimensional propagation of neutral quasiparticles. Their intrinsic properties, however, can be severely obscured by spatial energy fluctuations due to a high sensitivity to the immediate environment. Here, we take advantage of the encapsulation of individual layers in hexagonal boron nitride to strongly suppress environmental disorder. Diffusion of excitons is then directly monitored using time- and spatially-resolved emission microscopy at ambient conditions. We consistently find very efficient propagation with linear diffusion coefficients up to 10\,cm$^2$/s, corresponding to room temperature effective mobilities as high as 400\,cm$^2$/Vs as well as a correlation between rapid diffusion and short population lifetime. At elevated densities we detect distinct signatures of many-particle interactions and consequences of strongly suppressed Auger-like exciton-exciton annihilation. A combination of analytical and numerical theoretical approaches is employed to provide pathways towards comprehensive understanding of the observed linear and non-linear propagation phenomena. We emphasize the role of dark exciton states and present a mechanism for diffusion facilitated by free electron hole plasma from entropy-ionized excitons.

cond-mat.mes-hall↗

arXiv2019

Exciton propagation and halo formation in two-dimensional materials

The interplay of optics, dynamics and transport is crucial for the design of novel optoelectronic devices, such as photodetectors and solar cells. In this context, transition metal dichalcogenides (TMDs) have received much attention. Here, strongly bound excitons dominate optical excitation, carrier dynamics and diffusion processes. While the first two have been intensively studied, there is a lack of fundamental understanding of non-equilibrium phenomena associated with exciton transport that is of central importance e.g. for high efficiency light harvesting. In this work, we provide microscopic insights into the interplay of exciton propagation and many-particle interactions in TMDs. Based on a fully quantum mechanical approach and in excellent agreement with photoluminescence measurements, we show that Auger recombination and emission of hot phonons act as a heating mechanism giving rise to strong spatial gradients in excitonic temperature. The resulting thermal drift leads to an unconventional exciton diffusion characterized by spatial exciton halos.

cond-mat.mes-hall↗

arXiv2019

Intrinsic Lifetime of Higher Excitonic States in Tungsten Diselenide Monolayers

The reduced dielectric screening in atomically thin transition metal dichalcogenides allows to study the hydrogen-like series of higher exciton states in optical spectra even at room temperature. The width of excitonic peaks provides information about the radiative decay and phonon-assisted scattering channels limiting the lifetime of these quasi-particles. While linewidth studies so far have been limited to the exciton ground state, encapsulation with hBN has recently enabled quantitative measurements of the broadening of excited exciton resonances. Here, we present a joint experiment-theory study combining microscopic calculations with spectroscopic measurements on the intrinsic linewidth and lifetime of higher exciton states in hBN-encapsulated WSe$_2$ monolayers. Surprisingly, despite the increased number of scattering channels, we find both in theory and experiment that the linewidth of higher excitonic states is similar or even smaller compared to the ground state. Our microscopic calculations ascribe this behavior to a reduced exciton-phonon scattering efficiency for higher excitons due to spatially extended orbital functions.

cond-mat.mes-hall↗

arXiv2018

Spatial extent of the excited exciton states in WS$_2$ monolayers from diamagnetic shifts

We experimentally study the radii of excitons in hBN-encapsulated WS2 monolayers by means of magneto-optical reflectance spectroscopy at cryogenic temperatures in magnetic fields up to 29 T. We observe field-induced energy shifts of the exciton ground and excited states due to valley Zeeman and diamagnetic effects. We find the g factor of the first excited state of $-4.2(+/-0.1) to be essentially equal to that of the ground state of -4.35(+/-0.1). From diamagnetic shifts we determine the root mean square radii of the excitons. The radius of the first excited state is found to be 5-8 nm and that of the ground state around 2 nm. Our results further confirm the Wannier-Mott nature of the exciton quasiparticles in monolayer semiconductors and the assignment of the optical resonances in absorption-type measurements. They also provide additional support for the applicability of the effective mass hydrogenlike models in these systems.

cond-mat.mes-hall↗

arXiv2018

Dielectric Engineering of Electronic Correlations in a van der Waals Heterostructure

Heterostructures of van der Waals bonded layered materials offer unique means to tailor dielectric screening with atomic-layer precision, opening a fertile field of fundamental research. The optical analyses used so far have relied on interband spectroscopy. Here we demonstrate how a capping layer of hexagonal boron nitride (hBN) renormalizes the internal structure of excitons in a WSe$_2$ monolayer using intraband transitions. Ultrabroadband terahertz probes sensitively map out the full complex-valued mid-infrared conductivity of the heterostructure after optical injection of $1s$ A excitons. This approach allows us to trace the energies and linewidths of the atom-like $1s$-$2p$ transition of optically bright and dark excitons as well as the densities of these quasiparticles. The fundamental excitonic resonance red shifts and narrows in the WSe$_2$/hBN heterostructure compared to the bare monolayer. Furthermore, the ultrafast temporal evolution of the mid-infrared response function evidences the formation of optically dark excitons from an initial bright population. Our results provide key insight into the effect of non local screening on electron-hole correlations and open new possibilities of dielectric engineering of van der Waals heterostructures.

cond-mat.mtrl-sci↗

arXiv2018

Exciton diffusion and halo effects in monolayer semiconductors

We directly monitor exciton propagation in freestanding and SiO2-supported WS2 monolayers through spatially- and time-resolved micro-photoluminescence under ambient conditions. We find highly nonlinear behavior with characteristic, qualitative changes in the spatial profiles of the exciton emission and an effective diffusion coefficient increasing from 0.3 to more than 30 cm2/s, depending on the injected exciton density. Solving the diffusion equation while accounting for Auger recombination allows us to identify and quantitatively understand the main origin of the increase in the observed diffusion coefficient. At elevated excitation densities, the initial Gaussian distribution of the excitons evolves into long-lived halo shapes with micrometer-scale diameter, indicating additional memory effects in the exciton dynamics.

cond-mat.mes-hall↗