arXiv subjects

C. Schüller

Publications and source records attributed to C. Schüller.

At least 19 recordsLinked to original sources

arXiv2023

Charge transfer and asymmetric coupling of MoSe$_2$ valleys to the magnetic order of CrSBr

Van der Waals (vdW) heterostructures composed of two-dimensional (2D) transition metal dichalcogenides (TMD) and vdW magnetic materials offer an intriguing platform to functionalize valley and excitonic properties in non-magnetic TMDs. Here, we report magneto-photoluminescence (PL) investigations of monolayer (ML) MoSe$_2$ on the layered A-type antiferromagnetic (AFM) semiconductor CrSBr under different magnetic field orientations. Our results reveal a clear influence of the CrSBr magnetic order on the optical properties of MoSe$_2$, such as an anomalous linear-polarization dependence, changes of the exciton/trion energies, a magnetic-field dependence of the PL intensities, and a valley $g$-factor with signatures of an asymmetric magnetic proximity interaction. Furthermore, first principles calculations suggest that MoSe$_2$/CrSBr forms a broken-gap (type-III) band alignment, facilitating charge transfer processes. The work establishes that antiferromagnetic-nonmagnetic interfaces can be used to control the valley and excitonic properties of TMDs, relevant for the development of opto-spintronics devices.

cond-mat.mes-hall↗

arXiv2022

Valley-magnetophonon resonance for interlayer excitons

Heterobilayers consisting of MoSe$_2$ and WSe$_2$ monolayers can host optically bright interlayer excitons with intriguing properties such as ultralong lifetimes and pronounced circular polarization of their photoluminescence due to valley polarization, which can be induced by circularly polarized excitation or applied magnetic fields. Here, we report on the observation of an intrinsic valley-magnetophonon resonance for localized interlayer excitons promoted by invervalley hole scattering. It leads to a resonant increase of the photoluminescence polarization degree at the same field of 24.2 Tesla for H-type and R-type stacking configurations despite their vastly different excitonic energy splittings. As a microscopic mechanism of the hole intervalley scattering we identify the scattering with chiral TA phonons of MoSe$_2$ between excitonic states mixed by the long-range electron hole exchange interaction.

cond-mat.mes-hall↗

arXiv2021

Ultrafast charge-transfer dynamics in twisted MoS$_2$/WSe$_2$ heterostructures

Two-dimensional transition metal dichalcogenides (TMD) offer a unique platform for creating van-der-Waals heterojunctions with fascinating physical properties and promising applications in optoelectronics and valleytronics. Because of their typical type-II band alignment, photoexcited electrons and holes can separate via interfacial charge transfer. To understand the nature and the dynamics of this charge transfer is of utmost importance for the design and efficiency of potential devices. However, systematic studies concerning the influence of the stacking angle on the charge transfer remain sparse. Here, we apply time- and polarization resolved second-harmonic imaging microscopy to investigate the charge-transfer dynamics for three MoS$_2$/WSe$_2$ heterostructures with different stacking angles at a previously unattainable time-resolution of $\approx$ 6 fs. For 1.70 eV excitation energy, electron transfer from WSe$_2$ to MoS$_2$ is found to depend considerably on the stacking angle with the fastest transfer time observed to be as short as 12 fs. At 1.85 eV excitation energy, ultrafast hole transfer from MoS$_2$ to hybridized states at the $Γ$-point or to the K-points of WSe$_2$ has to be considered. Surprisingly, the corresponding decay dynamics show only a minor stacking-angle dependence indicating that radiative recombination of indirect $Γ$-K excitons becomes the dominant decay route for all samples.

cond-mat.mtrl-sci↗

arXiv2018

Asymmetric $g$ tensor in low-symmetry two-dimensional hole systems

The complex structure of the valence band in many semiconductors leads to multifaceted and unusual properties for spin-3/2 hole systems compared to typical spin-1/2 electron systems. In particular, two-dimensional hole systems show a highly anisotropic Zeeman spin splitting. We have investigated this anisotropy in GaAs/AlAs quantum well structures both experimentally and theoretically. By performing time-resolved Kerr rotation measurements, we found a non-diagonal tensor $g$ that manifests itself in unusual precessional motion as well as distinct dependencies of hole spin dynamics on the direction of the magnetic field $\vec{B}$. We quantify the individual components of the tensor $g$ for [113]-, [111]- and [110]-grown samples. We complement the experiments by a comprehensive theoretical study of Zeeman splitting in in-plane and out-of-plane fields $\vec{B}$. To this end, we develop a detailed multiband theory for the tensor $g$. Using perturbation theory, we derive transparent analytical expressions for the components of the tensor $g$ that we complement with accurate numerical calculations based on our theoretical framework. We obtain very good agreement between experiment and theory. Our study demonstrates that the tensor $g$ is neither symmetric nor antisymmetric. Opposite off-diagonal components can differ in size by up to an order of magnitude.

cond-mat.mes-hall↗

arXiv2017

Observation of macroscopic valley-polarized monolayer exciton-polaritons at room temperature

In this letter, we address the chiral properties of valley exciton-polaritons in a monolayer of WS2 in the regime of strong light-matter coupling with a Tamm-Plasmon resonance. We observe that the valley polarization, which manifests in the circular polarization of the emitted photoluminescence, is strongly enhanced in comparison to bare WS2 monolayers, and can even be observed under non-resonant excitation at ambient conditions. We study the relaxation and decay dynamics of exciton-polaritons in our device, and present a microscopic model to explain the wave vector-dependent valley depolarization as an interplay of bright and dark states, electron-hole exchange interaction and the linear polarization splitting inherent to the microcavity.

cond-mat.mes-hall↗

arXiv2017

Valley polarized relaxation and upconversion luminescence from Tamm-Plasmon Trion-Polaritons with a MoSe2 monolayer

Transition metal dichalcogenides represent an ideal testbed to study excitonic effects, spin-related phenomena and fundamental light-matter coupling in nanoscopic condensed matter systems. In particular, the valley degree of freedom, which is unique to such direct band gap monolayers with broken inversion symmetry, adds fundamental interest in these materials. Here, we implement a Tamm-plasmon structure with an embedded MoSe2 monolayer and study the formation of polaritonic quasi-particles. Strong coupling conditions between the Tamm-mode and the trion resonance of MoSe2 are established, yielding bright luminescence from the polaritonic ground state under non-resonant optical excitation. We demonstrate, that tailoring the electrodynamic environment of the monolayer results in a significantly increased valley polarization. This enhancement can be related to change in recombination dynamics shown in time-resolved photoluminescence measurements. We furthermore observe strong upconversion luminescence from resonantly excited polariton states in the lower polariton branch. This upconverted polariton luminescence is shown to preserve the valley polarization of the trion-polariton, which paves the way towards combining spin-valley physics and exciton scattering experiments.

cond-mat.mes-hall↗

arXiv2016

Coherent cyclotron motion beyond Kohn's theorem

In solids, the high density of charged particles makes many-body interactions a pervasive principle governing optics and electronics[1-12]. However, Walter Kohn found in 1961 that the cyclotron resonance of Landau-quantized electrons is independent of the seemingly inescapable Coulomb interaction between electrons[2]. While this surprising theorem has been exploited in sophisticated quantum phenomena[13-15] such as ultrastrong light-matter coupling[16], superradiance[17], and coherent control[18], the complete absence of nonlinearities excludes many intriguing possibilities, such as quantum-logic protocols[19]. Here, we use intense terahertz pulses to drive the cyclotron response of a two-dimensional electron gas beyond the protective limits of Kohn's theorem. Anharmonic Landau ladder climbing and distinct terahertz four- and six-wave mixing signatures occur, which our theory links to dynamic Coulomb effects between electrons and the positively charged ion background. This new context for Kohn's theorem unveils previously inaccessible internal degrees of freedom of Landau electrons, opening up new realms of ultrafast quantum control for electrons.

cond-mat.mes-hall↗

arXiv2016

Direct observation of internal quantum transitions and femtosecond radiative decay of excitons in monolayer WSe_2

Atomically thin two-dimensional crystals have revolutionized materials science. In particular, monolayer transition metal dichalcogenides promise novel optoelectronic applications, due to their direct energy gaps in the optical range. Their electronic and optical properties, however, are complicated by exotic room-temperature excitons, whose fundamental structure and dynamics has been under intense investigation. While interband spectroscopy probes energies of excitons with vanishing centre-of-mass momenta, the majority of excitons has remained elusive, raising questions about their unusual internal structure, symmetry, many-body effects, and dynamics. Here we report the first direct experimental access to all relevant excitons in single-layer WSe2. Phase-locked mid-infrared pulses reveal the internal orbital 1s-2p resonance, which is highly sensitive to the shape of the excitonic envelope functions and provides accurate transition energies, oscillator strengths, densities and linewidths. Remarkably, the observed decay dynamics indicates a record fast radiative annihilation of small-momentum excitons within 150 fs, whereas Auger recombination prevails for optically dark states. The results provide a comprehensive view of excitons and introduce a new degree of freedom for quantum control, optoelectronics and valleytronics of dichalcogenide monolayers.

cond-mat.mtrl-sci↗

arXiv2016

Ultrafast mid-infrared nanoscopy of strained vanadium dioxide nanobeams

Long regarded as a model system for studying insulator-to-metal phase transitions, the correlated electron material vanadium dioxide (VO$_2$) is now finding novel uses in device applications. Two of its most appealing aspects are its accessible transition temperature ($\sim$341 K) and its rich phase diagram. Strain can be used to selectively stabilize different VO$_2$ insulating phases by tuning the competition between electron and lattice degrees of freedom. It can even break the mesoscopic spatial symmetry of the transition, leading to a quasi-periodic ordering of insulating and metallic nanodomains. Nanostructuring of strained VO$_2$ could potentially yield unique components for future devices. However, the most spectacular property of VO$_2$ - its ultrafast transition - has not yet been studied on the length scale of its phase heterogeneity. Here, we use ultrafast near-field microscopy in the mid-infrared to study individual, strained VO$_2$ nanobeams on the 10 nm scale. We reveal a previously unseen correlation between the local steady-state switching susceptibility and the local ultrafast response to below-threshold photoexcitation. These results suggest that it may be possible to tailor the local photo-response of VO$_2$ using strain and thereby realize new types of ultrafast nano-optical devices.

cond-mat.mes-hall↗

arXiv2015

Control of biaxial strain in single-layer Molybdenite using local thermal expansion of the substrate

Single-layer MoS2 is a direct-gap semiconductor whose electronic band structure strongly depends on the strain applied to its crystal lattice. While uniaxial strain can be easily applied in a controlled way, e.g., by bending of a flexible substrate with the atomically thin MoS2 layer on top, experimental realization of biaxial strain is more challenging. Here, we exploit the large mismatch between the thermal expansion coefficients of MoS2 and a silicone-based substrate to apply a controllable biaxial tensile strain by heating the substrate with a focused laser. The effect of this biaxial strain is directly observable in optical spectroscopy as a redshift of the MoS2 photoluminescence. We also demonstrate the potential of this method to engineer more complex strain patterns by employing highly absorptive features on the substrate to achieve non-uniform heat profiles. By comparison of the observed redshift to strain-dependent band structure calculations, we estimate the biaxial strain applied by the silicone-based substrate to be up to 0.2 percent, corresponding to a band gap modulation of 105 meV per percentage of biaxial tensile strain.

cond-mat.mes-hall↗

arXiv2015

Optical spectroscopy of interlayer coupling in artificially stacked MoS2 layers

We perform an optical spectroscopy study to investigate the properties of different artificial MoS$_2$ bi- and trilayer stacks created from individual monolayers by a deterministic transfer process. These twisted bi- and trilayers differ from the common 2H stacking in mineral MoS$_2$ in the relative stacking angle of adjacent layers and the interlayer distance. The combination of Raman spectroscopy, second-harmonic-generation microscopy and photoluminescence measurements allows us to determine the degree of interlayer coupling in our samples. We find that even for electronically decoupled artificial structures, which show the same valley polarization degree as the constituent MoS$_2$ monolayers at low temperatures, there is a resonant energy transfer between individual layers which acts as an effective luminescence quenching mechanism.

cond-mat.mes-hall↗

arXiv2014

Hole spin dynamics and hole $g$ factor anisotropy in coupled quantum well systems

Due to its p-like character, the valence band in GaAs-based heterostructures offers rich and complex spin-dependent phenomena. One manifestation is the large anisotropy of Zeeman spin splitting. Using undoped, coupled quantum wells (QWs), we examine this anisotropy by comparing the hole spin dynamics for high- and low-symmetry crystallographic orientations of the QWs. We directly measure the hole $g$ factor via time-resolved Kerr rotation, and for the low-symmetry crystallographic orientations (110) and (113a), we observe a large in-plane anisotropy of the hole $g$ factor, in good agreement with our theoretical calculations. Using resonant spin amplification, we also observe an anisotropy of the hole spin dephasing in the (110)-grown structure, indicating that crystal symmetry may be used to control hole spin dynamics.

cond-mat.mes-hall↗

arXiv2013

A direct comparison of CVD-grown and exfoliated MoS2 using optical spectroscopy

MoS2 is a highly interesting material system, which exhibits a crossover from an indirect band gap in the bulk crystal to a direct gap for single layers. Here, we perform a direct comparison between large-area MoS$_2$ films grown by chemical vapor deposition (CVD) and MoS$_2$ flakes prepared by mechanical exfoliation from natural bulk crystal. Raman spectroscopy measurements show differences between the in-plane and out-of-plane phonon mode positions in CVD-grown and exfoliated MoS$_2$. Photoluminescence (PL) mapping reveals large regions in the CVD-grown films that emit strong PL at room temperature, and low-temperature PL scans demonstrate a large spectral shift of the A exciton emission as a function of position. Polarization-resolved PL measurements under near-resonant excitation conditions show a strong circular polarization of the PL, corresponding to a valley polarization.

cond-mat.mtrl-sci↗

arXiv2013

Spin dynamics in p-doped semiconductor nanostructures subject to a magnetic field tilted from the Voigt geometry

We develop a theoretical description of the spin dynamics of resident holes in a p-doped semiconductor quantum well (QW) subject to a magnetic field tilted from the Voigt geometry. We find the expressions for the signals measured in time-resolved Faraday rotation (TRFR) and resonant spin amplification (RSA) experiments and study their behavior for a range of system parameters. We find that an inversion of the RSA peaks can occur for long hole spin dephasing times and tilted magnetic fields. We verify the validity of our theoretical findings by performing a series of TRFR and RSA experiments on a p-modulation doped GaAs/Al_{0.3}Ga_{0.7}As single QW and showing that our model can reproduce experimentally observed signals.

cond-mat.mes-hall↗

arXiv2012

Anisotropic spin relaxation revealed by resonant spin amplification in (110) GaAs quantum wells

We have studied spin dephasing in a high-mobility two-dimensional electron system (2DES), confined in a GaAs/AlGaAs quantum well grown in the [110] direction, using the resonant spin amplification (RSA) technique. From the characteristic shape of the RSA spectra, we are able to extract the spin dephasing times (SDT) for electron spins aligned along the growth direction or within the sample plane, as well as the $g$ factor. We observe a strong anisotropy in the spin dephasing times. While the in-plane SDT remains almost constant as the temperature is varied between 4 K and 50 K, the out-of-plane SDT shows a dramatic increase at a temperature of about 25 K and reaches values of about 100 ns. The SDTs at 4 K can be further increased by additional, weak above-barrier illumination. The origin of this unexpected behavior is discussed, the SDT enhancement is attributed to the redistribution of charge carriers between the electron gas and remote donors.

cond-mat.mtrl-sci↗

arXiv2012

Decoherence-assisted initialization of a resident hole spin polarization in a two-dimensional hole gas

We investigate spin dynamics of resident holes in a p-modulation-doped GaAs/Al$_{0.3}$Ga$_{0.7}$As single quantum well. Time-resolved Faraday and Kerr rotation, as well as resonant spin amplification, are utilized in our study. We observe that nonresonant or high power optical pumping leads to a resident hole spin polarization with opposite sign with respect to the optically oriented carriers, while low power resonant optical pumping only leads to a resident hole spin polarization if a sufficient in-plane magnetic field is applied. The competition between two different processes of spin orientation strongly modifies the shape of resonant spin amplification traces. Calculations of the spin dynamics in the electron--hole system are in good agreement with the experimental Kerr rotation and resonant spin amplification traces and allow us to determine the hole spin polarization within the sample after optical orientation, as well as to extract quantitative information about spin dephasing processes at various stages of the evolution.

cond-mat.mes-hall↗

arXiv2012

Low-temperature photoluminescence of oxide-covered single-layer MoS2

We present a photoluminescence study of single-layer MoS2 flakes on SiO2 surfaces. We demonstrate that the luminescence peak position of flakes prepared from natural MoS2, which varies by up to 25 meV between individual as-prepared flakes, can be homogenized by annealing in vacuum, which removes adsorbates from the surface. We use HfO2 and Al2O3 layers prepared by atomic layer deposition to cover some of our flakes. We clearly observe a suppression of the low-energy luminescence peak observed for as-prepared flakes at low temperatures, indicating that this peak originates from excitons bound to surface adsorbates. We also observe different temperature-induced shifts of the luminescence peaks for the oxide-covered flakes. This effect stems from the different thermal expansion coefficients of the oxide layers and the MoS2 flakes. It indicates that the single-layer MoS2 flakes strongly adhere to the oxide layers and are therefore strained.

cond-mat.mtrl-sci↗

arXiv2011

Low-temperature photocarrier dynamics in monolayer MoS2

The band structure of MoS$_2$ strongly depends on the number of layers, and a transition from indirect to direct-gap semiconductor has been observed recently for a single layer of MoS$_2$. Single-layer MoS$_2$ therefore becomes an efficient emitter of photoluminescence even at room temperature. Here, we report on scanning Raman and on temperature-dependent, as well as time-resolved photoluminescence measurements on single-layer MoS$_2$ flakes prepared by exfoliation. We observe the emergence of two distinct photoluminescence peaks at low temperatures. The photocarrier recombination at low temperatures occurs on the few-picosecond timescale, but with increasing temperatures, a biexponential photoluminescence decay with a longer-lived component is observed.

cond-mat.mtrl-sci↗