Fabian Mooshammer

Femtosecond photo-switching of interface polaritons in black phosphorus heterostructures

The possibility of hybridizing collective electronic motion with mid-infrared light to form surface polaritons has made van der Waals layered materials a versatile platform for extreme light confinement and tailored nanophotonics. Graphene and its heterostructures have attracted particular attention because the absence of an energy gap allows plasmon polaritons to be tuned continuously. Here, we introduce black phosphorus as a promising new material in surface polaritonics that features key advantages for ultrafast switching. Unlike graphene, black phosphorus is a van der Waals bonded semiconductor, which enables high-contrast interband excitation of electron-hole pairs by ultrashort near-infrared pulses. Here, we design a SiO2/black phosphorus/SiO2 heterostructure in which the surface phonon modes of the SiO2 layers hybridize with surface plasmon modes in black phosphorus that can be activated by photo-induced interband excitation. Within the Reststrahlen band of SiO2, the hybrid interface polariton assumes surface-phonon-like properties, with a well-defined frequency and momentum and excellent coherence. During the lifetime of the photogenerated electron-hole plasma, coherent hybrid polariton waves can be launched by a broadband mid-infrared pulse coupled to the tip of a scattering-type scanning near-field optical microscopy set-up. The scattered radiation allows us to trace the new hybrid mode in time, energy and space. We find that the surface mode can be activated within ∼50 fs and disappears within 5 ps, as the electron-hole pairs in black phosphorus recombine. The excellent switching contrast and switching speed, the coherence properties and the constant wavelength of this transient mode make it a promising candidate for ultrafast nanophotonic devices.

Giant magnetic 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 artificial design of a two-dimensional heterostructure enabling intervalley transitions that are not accessible in monolayer systems. The resulting giant effective g factor of −15 for interlayer excitons induces near-unity valley polarization via valley-selective energetic splitting in high magnetic fields, even after nonselective excitation. Our results highlight the potential to deterministically engineer novel valley properties in van der Waals heterostructures using crystallographic alignment.In transition metal dichalcogenide monolayers, the spin and valley degrees of freedom are strongly coupled. Here, the authors engineer a WSe2/MoSe2 heterostructure in which inter-valley transitions of interlayer excitons exhibit a giant splitting and near-unity polarization in a magnetic field.

Momentum-space indirect interlayer excitons in transition-metal dichalcogenide van der Waals heterostructures

Monolayers of transition-metal dichalcogenides feature exceptional optical properties that are dominated by tightly bound electron–hole pairs, called excitons. Creating van der Waals heterostructures by deterministically stacking individual monolayers can tune various properties via the choice of materials1 and the relative orientation of the layers2,3. In these structures, a new type of exciton emerges where the electron and hole are spatially separated into different layers. These interlayer excitons4–6 allow exploration of many-body quantum phenomena7,8 and are ideally suited for valleytronic applications9. A basic model of a fully spatially separated electron and hole stemming from the K valleys of the monolayer Brillouin zones is usually applied to describe such excitons. Here, we combine photoluminescence spectroscopy and first-principles calculations to expand the concept of interlayer excitons. We identify a partially charge-separated electron–hole pair in MoS2/WSe2 heterostructures where the hole resides at the Γ point and the electron is located in a K valley. We control the emission energy of this new type of momentum-space indirect, yet strongly bound exciton by variation of the relative orientation of the layers. These findings represent a crucial step towards the understanding and control of excitonic effects in van der Waals heterostructures and devices.A new type of exciton is observed in transition-metal dichalcogenide heterobilayers that is indirect in both real space and momentum space. It consists of a paired electron in MoS2 at the K point and hole spread across MoS2 and WSe2 at the Γ point.

Optical spectroscopy of interlayer excitons in TMDC heterostructures: exciton dynamics, interactions, and giant valley-selective magnetic splitting

Two-dimensional transition-metal dichalcogenides (TMDCs) have recently emerged as a promising class of materials. A fascinating aspect of these atomically thin crystals is the possibility of combining different TMDCs into heterostructures. For several TMDC combinations, a staggered band alignment occurs, so that optically excited electron-hole pairs are spatially separated into different layers and form interlayer excitons (IEX). Here, we report on time-resolved, low-temperature photoluminescence (PL) of these IEX in a MoSe2-WSe2 heterostructure. In the time-resolved measurements, we observe indications of IEX diffusion in an inhomogeneous potential landscape. Excitation-density-dependent measurements reveal a dipolar, repulsive exciton-exciton interaction. PL measurements in applied magnetic fields show a giant valley-selective splitting of the IEX luminescence, with an effective g factor of about -15. This large value stems from the alignment of K+ and K- valleys of the constituent monolayers in our heterostructure, making intervalley transitions optically bright, so that contributions to the field-induced splitting arising from electron and hole valley magnetic moments add up. This giant splitting enables us to generate a near-unity valley polarization of interlayer excitons even under linearly polarized excitation by applying sufficiently large magnetic fields.

Ultrafast photo-activation of interface polaritons in black phosphorus heterostructures

Van der Waals layered materials, such as graphene, hexagonal boron nitride, and transition metal dichalcogenides, have redefined the perspectives of future ultra-compact electronics and optics on the nanoscale. Specifically, the possibility of hybridizing collective electronic motion with mid-infrared photons in so-called surface polaritons has allowed for extreme light confinement and represents a key ingredient for tailored nanophotonics [1].

Optical spectroscopy of valley dynamics and interlayer excitons in transition-metal dichalcogenide monolayers and heterostructures

Monolayer transition-metal dichalcogenides (TMDs) have recently emerged as fascinating novel materials. Like graphene, they can easily be exfoliated from bulk crystals. Unlike graphene, they have a large and direct band gap, making them attractive for potential applications in electronics or optoelectronics. They may also allow for novel device functionalities, as the spin and valley pseudospin degrees of freedom are directly coupled and stabilized by a large spin splitting in the conduction and valence bands. The optical properties of these two-dimensional crystals are dominated by tightly bound electron-hole pairs (excitons) and more complex quasiparticles such as charged excitons (trions) and biexcitons.

Terahertz subcycle control: From high-harmonic generation to molecular snapshots

Atomically strong THz fields accelerate electrons in bulk semiconductors, new 2D materials, and atomically sharp tunneling junctions. By tracking this lightwave-driven charge transport with subcycle resolution, we explore dynamical Bloch oscillations as well as quasiparticle collisions and record the first single-molecule femtosecond movie.

Terahertz imaging with ultimate resolution

Summary form only given. Field-resolved detection of ultrafast pulses in the THz (0.1-10 THz) and multi-THz (10-100 THz) spectral range has provided key insights into the dynamics of low-energy collective excitations in condensed matter systems. However, the spatial resolution of these far-field studies is intrinsically limited to the scale of the probing wavelength by diffraction. Thus, the measured optical response is an average over sub-wavelength structures such as nanoparticles, nanocrystals, nanodomains, and microscopic defects. Apertureless scattering-type near-field scanning optical microscopy (s-NSOM) bypasses this fundamental limit by utilizing the strong confinement of the optical near-field at the apex of a sharp metal tip. We have combined ultra-sensitive, field-resolved multi-THz spectroscopy with s-NSOM to access dynamic complex conductivities on the surfaces of nanostructures with 10 nm spatial resolution. Electro-optic sampling of the scattered near-field pulses enables sub-cycle detection (10 fs temporal resolution) of waveforms consisting of less than one coherent photon per pulse. We have applied our versatile microscope to two nanostructures of similar shape but vastly different composition. First, carrier dynamics were studied in indium arsenide nanowires with sub-cycle temporal resolution, revealing the ultrafast (<; 50 fs) formation of a carrier depletion layer at the nanowire surface. Second, we studied heterogeneous local dynamics in vanadium dioxide nanowires. Vanadium dioxide is a model system for insulator-to-metal phase transitions and is promising for technological applications. In our study, we found that substrate-induced strain drives a periodic modulation of the ultrafast photoconductivity along the nanowire. Finally, we have explored the ultimate limits of THz imaging resolution using a new technique called THz scanning tunnelling microscopy, where THz pulses drive femtosecond local currents across an atomic-scale tunnel junction.