arXiv subjects

Christian Schüller

Publications and source records attributed to Christian Schüller.

At least 37 records · Page 2Linked to original sources

arXiv2017

Characterization of highly crystalline lead iodide nanosheets prepared by room-temperature solution processing

Two-dimensional semiconducting materials are particularly appealing for many applications. Although theory predicts a large number of two-dimensional materials, experimentally only a few of these materials have been identified and characterized comprehensively in the ultrathin limit. Lead iodide, which belongs to the transition metal halides family and has a direct bandgap in the visible spectrum, has been known for a long time and has been well characterized in its bulk form. Nevertheless, studies of this material in the nanometer thickness regime are rather scarce. In this article we demonstrate an easy way to synthesize ultrathin, highly crystalline flakes of PbI2 by precipitation from a solution in water. We thoroughly characterize the produced thin flakes with different techniques ranging from optical and Raman spectros-copy to temperature-dependent photoluminescence and electron microscopy. We compare the results to ab initio calculations of the band structure of the material. Finally, we fabricate photodetectors based on PbI2 and study their optoelectronic properties.

cond-mat.mes-hall↗

arXiv2017

Valley Dynamics of Excitons in Monolayer Dichalcogenides

Monolayer transition-metal dichalcogenides (TMDCs) have recently emerged as possible candidates for valleytronic applications, as the spin and valley pseudospin are directly coupled and stabilized by a large spin splitting. In these semiconducting materials, optically excited electron-hole pairs form tightly Coulomb-bound excitons with large binding energies. The selection rules for excitonic transitions allow for direct optical generation of a valley-polarized exciton population using resonant excitation. Here, we investigate the exciton valley dynamics in monolayers of three different TMDCs by means of time-resolved Kerr rotation at low temperatures. We observe pronounced differences in the valley dynamics of tungsten- and molybdenum-based TMDCs, which are directly related to the opposite order of the conduction-band spin splitting in these materials.

cond-mat.mes-hall↗

arXiv2017

Long-lived spin polarization in n-doped MoSe$_2$ monolayers

Transition metal dichalcogenide monolayers are highly interesting for potential valleytronic applications due to the coupling of spin and valley degrees of freedom and valley-selective excitonic transitions. However, ultrafast recombination of excitons in these materials poses a natural limit for applications, so that a transfer of polarization to resident carriers is highly advantageous. Here, we study the low-temperature spin-valley dynamics in nominally undoped and n-doped MoSe$_2$ monolayers using time-resolved Kerr rotation. In the n-doped MoSe$_2$, we find a long-lived component of the Kerr signal which we attribute to the spin polarization of resident carriers. This component is absent in the nominally undoped MoSe$_2$. The long-lived spin polarization is stable under applied in-plane magnetic fields. Spatially resolved measurements allow us to determine an upper boundary for the electron spin diffusion constant in MoSe$_2$.

cond-mat.mes-hall↗

arXiv2017

Giant Zeeman splitting inducing near-unity valley polarization in van der Waals heterostructures

Monolayers of semiconducting transition metal dichalcogenides exhibit intriguing fundamental physics of strongly coupled spin and valley degrees of freedom for charge carriers. While the possibility of exploiting these properties for information processing stimulated concerted research activities towards the concept of valleytronics , maintaining control over spin-valley polarization proved challenging in individual monolayers. A promising alternative route explores type II band alignment in artificial van der Waals heterostructures. The resulting formation of interlayer excitons combines the advantages of long carrier lifetimes and spin-valley locking . Here, we demonstrate direct magnetic manipulation of valley polarization in a WSe2/MoSe2 heterostructure through giant valley Zeeman splitting of interlayer transitions. Remarkably, even after non-selective injection, the observed $g$ factor as large as $-15$ induces near-unity polarization of long-lived excitons with 100 ns lifetimes under magnetic fields. The demonstrated control of the spin-valley physics highlights the exceptional aspects of novel, artificially designed material systems and their promise for atomically-thin valleytronic devices.

cond-mat.mes-hall↗

arXiv2017

Polarized SERS of individual suspended carbon nanotubes by Pt-Re nanoantennas

We present optical nanoantennas designed for applications that require processing temperatures larger than 800°C. The antennas consist of arrays of Re/Pt bilayer strips fabricated with a lift-off-free technique on top of etched trenches. Reflectance measurements show a clear plasmonic resonance at approximately 670 nm for light polarized orthogonal to the strip axis. The functionality of the antennas is demonstrated by growing single-walled carbon nanotubes (CNTs) on top of the antenna arrays and measuring the corresponding Raman signal enhancement of individual CNTs. The results of the measurements are quantitatively discussed in light of numerical simulations which highlight the impact of the substrate.

cond-mat.mes-hall↗

arXiv2017

Interlayer exciton dynamics in a dichalcogenide monolayer heterostructure

In heterostructures consisting of different transition-metal dichalcogenide monolayers, a staggered band alignment can occur, leading to rapid charge separation of optically generated electron-hole pairs into opposite monolayers. These spatially separated electron-hole pairs are Coulomb-coupled and form interlayer excitons. Here, we study these interlayer excitons in a heterostructure consisting of MoSe$_2$ and WSe$_2$ monolayers using photoluminescence spectroscopy. We observe a non-trivial temperature dependence of the linewidth and the peak energy of the interlayer exciton, including an unusually strong initial redshift of the transition with temperature, as well as a pronounced blueshift of the emission energy with increasing excitation power. By combining these observations with time-resolved photoluminescence measurements, we are able to explain the observed behavior as a combination of interlayer exciton diffusion and dipolar, repulsive exciton-exciton interaction.

cond-mat.mes-hall↗

arXiv2017

Direct observation of the band gap transition in atomically thin ReS$_2$

ReS$_2$ is considered as a promising candidate for novel electronic and sensor applications. The low crystal symmetry of the van der Waals compound ReS$_2$ leads to a highly anisotropic optical, vibrational, and transport behavior. However, the details of the electronic band structure of this fascinating material are still largely unexplored. We present a momentum-resolved study of the electronic structure of monolayer, bilayer, and bulk ReS$_2$ using k-space photoemission microscopy in combination with first-principles calculations. We demonstrate that the valence electrons in bulk ReS$_2$ are - contrary to assumptions in recent literature - significantly delocalized across the van der Waals gap. Furthermore, we directly observe the evolution of the valence band dispersion as a function of the number of layers, revealing a significantly increased effective electron mass in single-layer crystals. We also find that only bilayer ReS$_2$ has a direct band gap. Our results establish bilayer ReS$_2$ as a advantageous building block for two-dimensional devices and van der Waals heterostructures.

cond-mat.mtrl-sci↗

arXiv2017

Spectral focusing of broadband silver electroluminescence in nanoscopic FRET-LEDs

Few inventions have shaped the world like the incandescent bulb. While Edison used thermal radiation from ohmically heated conductors, some noble metals exhibit "cold" electroluminescence (EL) in percolation films, tunnel diodes, electromigrated nanoparticle aggregates, optical antennae, or scanning-tunnelling microscopy (STM). The origin of this radiation, which is spectrally broad and depends on applied bias, is controversial given the low radiative yields of electronic transitions. Nanoparticle EL is particularly intriguing since it involves localized surface-plasmon resonances with large dipole moments. Such plasmons enable very efficient non-radiative fluorescence resonance energy transfer (FRET) coupling to proximal resonant dipole transitions. We demonstrate nanoscopic FRET-LEDs which exploit the opposite process, energy transfer from silver nanoparticles to exfoliated monolayers of transition-metal dichalcogenides (TMDCs). In diffraction-limited hotspots showing pronounced photon bunching, broadband silver EL is focused into the narrow excitonic resonance of the atomically thin overlayer. Such devices may offer alternatives to conventional nano-LEDs in on-chip optical interconnects.

physics.optics↗

arXiv2017

Coulomb engineering of the bandgap in 2D semiconductors

The ability to control the size of the electronic bandgap is an integral part of solid-state technology. Atomically-thin two-dimensional crystals offer a new approach for tuning the energies of the electronic states based on the interplay between the environmental sensitivity and unusual strength of the Coulomb interaction in these materials. By engineering the surrounding dielectric environment, we are able to tune the electronic bandgap in monolayers of WS2 and WSe2 by hundreds of meV. We exploit this behavior to present an in-plane dielectric heterostructure with a spatially dependent bandgap, illustrating the feasibility of our approach for the creation of lateral junctions with nanoscale resolution. This successful demonstration of bandgap engineering based on the non-invasive modification of the Coulomb interaction should enable the design of a new class of atomically thin devices to advance the limits of size and functionality for solid-state technologies.

cond-mat.mes-hall↗

arXiv2016

Excitonic valley effects in monolayer WS$_2$ under high magnetic fields

Transition-metal dichalcogenides can be easily produced as atomically thin sheets, exhibiting the possibility to optically polarize and read out the valley pseudospin of extremely stable excitonic quasiparticles present in these 2D semiconductors. Here, we investigate a monolayer of tungsten disulphide in high magnetic fields up to 30\,T via photoluminescence spectroscopy at low temperatures. The valley degeneracy is lifted for all optical features, particularly for excitons, singlet and triplet trions, for which we determine the g factor separately. While the observation of a diamagnetic shift of the exciton and trion resonances gives us insight into the real-space extension of these quasiparticles, magnetic field induced valley polarization effects shed light onto the exciton and trion dispersion relations in reciprocal space. The field dependence of the trion valley polarizations is in line with the predicted trion splitting into singlet and triplet configurations.

cond-mat.mes-hall↗

arXiv2016

Trion Valley Coherence in Monolayer Semiconductors

The emerging field of valleytronics aims to exploit the valley pseudospin of electrons residing near Bloch band extrema as an information carrier. Recent experiments demonstrating optical generation and manipulation of exciton valley coherence (the superposition of electron-hole pairs at opposite valleys) in monolayer transition metal dichalcogenides (TMDs) provide a critical step towards control of this quantum degree of freedom. The charged exciton (trion) in TMDs is an intriguing alternative to the neutral exciton for control of valley pseudospin because of its long spontaneous recombination lifetime, its robust valley polarization, and its coupling to residual electronic spin. Trion valley coherence has however been unexplored due to experimental challenges in accessing it spectroscopically. In this work, we employ ultrafast two-dimensional coherent spectroscopy to resonantly generate and detect trion valley coherence in monolayer MoSe$_2$ demonstrating that it persists for a few-hundred femtoseconds. We conclude that the underlying mechanisms limiting trion valley coherence are fundamentally different from those applicable to exciton valley coherence. Based on these observations, we suggest possible strategies for extending valley coherence times in two-dimensional materials.

cond-mat.mes-hall↗

arXiv2016

Neutral and Charged Inter-Valley Biexcitons in Monolayer MoSe$_2$

In atomically thin transition metal dichalcogenides (TMDs), reduced dielectric screening of the Coulomb interaction leads to strongly correlated many-body states, including excitons and trions, that dominate the optical properties. Higher-order states, such as bound biexcitons, are possible but are difficult to identify unambiguously using linear optical spectroscopy methods alone. Here, we implement polarization-resolved two-dimensional coherent spectroscopy to unravel the complex optical response of monolayer MoSe$_2$ and identify multiple higher-order correlated states. Decisive signatures of neutral and charged inter-valley biexcitons appear in cross-polarized two-dimensional spectra as distinct resonances with respective ~20 meV and ~5 meV binding energies--similar to recent calculations using variational and Monte Carlo methods. A theoretical model taking into account the valley-dependent optical selection rules reveals the specific quantum pathways that give rise to these states. Inter-valley biexcitons identified here, comprised of neutral and charged excitons from different valleys, offer new opportunities for creating exotic exciton-polariton condensates and for developing ultrathin biexciton lasers and polarization-entangled photon sources.

cond-mat.mes-hall↗

arXiv2016

Enhanced spin-orbit coupling in core/shell nanowires

The spin-orbit coupling (SOC) in semiconductors is strongly influenced by structural asymmetries, as prominently observed in bulk crystal structures that lack inversion symmetry. Here, we study an additional effect on the SOC: the asymmetry induced by the large interface area between a nanowire core and its surrounding shell. Our experiments on purely wurtzite GaAs/AlGaAs core/shell nanowires demonstrate optical spin injection into a single free-standing nanowire and determine the effective electron g-factor of the hexagonal GaAs wurtzite phase. The spin relaxation is highly anisotropic in time-resolved micro-photoluminescence measurements on single nanowires, showing a significant increase of spin relaxation in external magnetic fields. This behavior is counterintuitive compared to bulk wurtzite crystals. We present a model for the observed electron spin dynamics highlighting the dominant role of the interface-induced SOC in these core/shell nanowires. This enhanced SOC may represent an interesting tuning parameter for the implementation of spin-orbitronic concepts in semiconductor-based structures.

cond-mat.mes-hall↗

arXiv2016

Coherent and Incoherent Coupling Dynamics between Neutral and Charged Excitons in Monolayer MoSe2

The optical properties of semiconducting transition metal dichalcogenides are dominated by both neutral excitons (electron-hole pairs) and charged excitons (trions) that are stable even at room temperature. While trions directly influence charge transport properties in optoelectronic devices, excitons may be relevant through exciton-trion coupling and conversion phenomena. In this work, we reveal the coherent and incoherent nature of exciton-trion coupling and the relevant timescales in monolayer MoSe2 using optical two-dimensional coherent spectroscopy. Coherent interaction between excitons and trions is definitively identified as quantum beating of cross-coupling peaks that persists for a few hundred femtoseconds. For longer times up to 10 ps, surprisingly, the relative intensity of the cross-coupling peaks increases, which is attributed to incoherent energy transfer likely due to phonon-assisted up-conversion and down-conversion processes that are efficient even at cryogenic temperature.

cond-mat.mes-hall↗

arXiv2016

Excitonic linewidth and coherence lifetime in monolayer transition metal dichalcogenides

Atomically thin transition metal dichalcogenides (TMDs) are direct-gap semiconductors with strong light-matter and Coulomb interaction. The latter accounts for tightly bound excitons, which dominate the optical properties of these technologically promising materials. Besides the optically accessible bright excitons, these systems exhibit a variety of dark excitonic states. They are not visible in optical spectra, but can strongly influence the coherence lifetime and the linewidth of the emission from bright exciton states. In a recent study, an experimental evidence for the existence of such dark states has been demonstrated, as well as their strong impact on the quantum efficiency of light emission in TMDs. Here, we reveal the microscopic origin of the excitonic coherence lifetime in two representative TMD materials (WS$_2$ and MoSe$_2$) within a joint study combining microscopic theory with optical experiments. We show that the excitonic coherence lifetime is determined by phonon-induced intra- and intervalley scattering into dark excitonic states. Remarkably, and in accordance with the theoretical prediction, we find an efficient exciton relaxation in WS$_2$ through phonon emission at all temperatures.

cond-mat.mtrl-sci↗

arXiv2015

Observation of anisotropic interlayer Raman modes in few-layer ReS2

ReS$_2$ has recently emerged as a new member in the rapidly growing family of two-dimensional materials. Unlike MoS$_2$ or WSe$_2$, the optical and electrical properties of ReS$_2$ are not isotropic due to the reduced symmetry of the crystal. Here, we present layer-dependent Raman measurements of ReS$_2$ samples ranging from monolayers to ten layers in the ultralow frequency regime. We observe layer breathing and shear modes which allow for easy assignment of the number of layers. Polarization-dependent measurements give further insight into the crystal structure and reveal an energetic shift of the shear mode which stems from the in-plane anisotropy of the shear modulus in this material.

cond-mat.mes-hall↗

arXiv2015

Identification of excitons, trions and biexcitons in single-layer WS2

Single-layer WS$_2$ is a direct-gap semiconductor showing strong excitonic photoluminescence features in the visible spectral range. Here, we present temperature-dependent photoluminescence measurements on mechanically exfoliated single-layer WS$_2$, revealing the existence of neutral and charged excitons at low temperatures as well as at room temperature. By applying a gate voltage, we can electrically control the ratio of excitons and trions and assert a residual n-type doping of our samples. At high excitation densities and low temperatures, an additional peak at energies below the trion dominates the photoluminescence, which we identify as biexciton emission.

cond-mat.mes-hall↗

arXiv2015

Tailored nano-antennas for directional Raman studies of individual carbon nanotubes

We exploit the near field enhancement of nano-antennas to investigate the Raman spectra of otherwise not optically detectable carbon nanotubes (CNTs). We demonstrate that a top-down fabrication approach is particularly promising when applied to CNTs, owing to the sharp dependence of the scattered intensity on the angle between incident light polarization and CNT axis. In contrast to tip enhancement techniques, our method enables us to control the light polarization in the sample plane, locally amplifying and rotating the incident field and hence optimizing the Raman signal. Such promising features are confirmed by numerical simulations presented here. The relative ease of fabrication and alignment makes this technique suitable for the realization of integrated devices that combine scanning probe, optical, and transport characterization.

cond-mat.mes-hall↗