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Maximilian Heithoff

Publications and source records attributed to Maximilian Heithoff.

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Localized emission in MoSe$_2$ monolayers on GaN nanopillars

Solid-state quantum emitters (QEs) in two-dimensional semiconductors offer compact, chip-compatible sources for quantum photonics. In transition-metal dichalcogenides (TMDs), nanopillars are widely used to induce localized emission, yet the underlying confinement mechanism and the relative roles of strain versus dielectric environment remain unclear. The general problem addressed here is whether strain alone explains quantum emitter formation and placement in MoSe$_2$, or whether dielectric contrast at suspended-supported interfaces is also required. Here, we combine hyperspectral superlocalization of photoluminescence with co-registered AFM topography and phase to map the positions of localized states (LS) in MoSe$_2$ suspended on GaN pillars and correlate them with bending strain and the local dielectric context. Contrary to the common assumption of purely strain-driven activation, LS frequently occur at suspended--supported interfaces around the pillar apex and span a broad strain range without a clear threshold, while being scarce along high-strain ripples. Our data indicate that deterministic emitter positioning in Mo-based TMDs benefits from co-engineering both strain gradients and nanoscale dielectric heterogeneity, rather than strain alone. More broadly, this combined optical-mechanical characterization approach provides a general framework for mapping structure-property relationships in 2D quantum materials at the single-emitter level.

cond-mat.mes-hall

Valley-hybridized gate-tunable 1D exciton confinement in MoSe2

Controlling excitons at the nanoscale in semiconductor materials represents a formidable challenge in the fields of quantum photonics and optoelectronics. Achieving this control holds great potential for unlocking strong exciton-exciton interaction regimes, enabling exciton-based logic operations, exploring exotic quantum phases of matter, facilitating deterministic positioning and tuning of quantum emitters, and designing advanced optoelectronic devices. Monolayers of transition metal dichalcogenides (TMDs) offer inherent two-dimensional confinement and possess significant binding energies, making them particularly promising candidates for achieving electric-field-based confinement of excitons without dissociation. While previous exciton engineering strategies have predominantly focused on local strain gradients, the recent emergence of electrically confined states in TMDs has paved the way for novel approaches. Exploiting the valley degree of freedom associated with these confined states further broadens the prospects for exciton engineering. Here, we show electric control of light polarization emitted from one-dimensional (1D) quantum confined states in MoSe2. By employing non-uniform in-plane electric fields, we demonstrate the in-situ tuning of the trapping potential and reveal how gate-tunable valley-hybridization gives rise to linearly polarized emission from these localized states. Remarkably, the polarization of the localized states can be entirely engineered through either the spatial geometry of the 1D confinement potential or the application of an out-of-plane magnetic field.

cond-mat.mes-hall

Valley lifetimes of conduction band electrons in monolayer WSe$_2$

One of the main tasks in the investigation of 2-dimensional transition metal dichalcogenides is the determination of valley lifetimes. In this work, we combine time-resolved Kerr rotation with electrical transport measurements to explore the gate-dependent valley lifetimes of free conduction band electrons of monolayer WSe$_2$. When tuning the Fermi energy into the conduction band we observe a strong decrease of the respective valley lifetimes which is consistent with both spin-orbit and electron-phonon scattering. We explain the formation of a valley polarization by the scattering of optically excited valley polarized bright trions into dark states by intervalley scattering. Furthermore, we show that the conventional time-resolved Kerr rotation measurement scheme has to be modified to account for photo-induced gate screening effects. Disregarding this adaptation can lead to erroneous conclusions drawn from gate-dependent optical measurements and can completely mask the true gate-dependent valley dynamics.

cond-mat.mes-hall

Unveiling valley lifetimes of free charge carriers in monolayer WSe$_2$

We report on nanosecond long, gate-dependent valley lifetimes of free charge carriers in monolayer WSe$_2$, unambiguously identified by the combination of time-resolved Kerr rotation and electrical transport measurements. While the valley polarization increases when tuning the Fermi level into the conduction or valence band, there is a strong decrease of the respective valley lifetime consistent with both electron-phonon and spin-orbit scattering. The longest lifetimes are seen for spin-polarized bound excitons in the band gap region. We explain our findings via two distinct, Fermi level-dependent scattering channels of optically excited, valley polarized bright trions either via dark or bound states. By electrostatic gating we demonstrate that the transition metal dichalcogenide WSe$_2$ can be tuned to be either an ideal host for long-lived localized spin states or allow for nanosecond valley lifetimes of free charge carriers (> 10 ns).

cond-mat.mes-hall

Spin States Protected from Intrinsic Electron-Phonon-Coupling Reaching 100 ns Lifetime at Room Temperature in MoSe$_2$

We present time-resolved Kerr rotation measurements, showing spin lifetimes of over 100 ns at room temperature in monolayer MoSe$_2$. These long lifetimes are accompanied by an intriguing temperature dependence of the Kerr amplitude, which increases with temperature up to 50 K and then abruptly switches sign. Using ab initio simulations we explain the latter behavior in terms of the intrinsic electron-phonon coupling and the activation of transitions to secondary valleys. The phonon-assisted scattering of the photo-excited electron-hole pairs prepares a valley spin polarization within the first few ps after laser excitation. The sign of the total valley magnetization, and thus the Kerr amplitude, switches as a function of temperature, as conduction and valence band states exhibit different phonon-mediated inter-valley scattering rates. However, the electron-phonon scattering on the ps time scale does not provide an explanation for the long spin lifetimes. Hence, we deduce that the initial spin polarization must be transferred into spin states which are protected from the intrinsic electron-phonon coupling, and are most likely resident charge carriers which are not part of the itinerant valence or conduction band states.

cond-mat.mes-hall