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Caspar H. van der Wal

Publications and source records attributed to Caspar H. van der Wal.

At least 19 recordsLinked to original sources
arXiv2026

Quantum communication networks with defects in silicon carbide

Quantum communication promises unprecedented capabilities enabled by the transmission of quantum states of light. However, current implementations face severe distance limitations due to photon loss. Silicon carbide (SiC) defects have emerged as a promising quantum device platform, offering strong optical transitions, long spin coherence lifetimes and the opportunity for integration with semiconductor devices. Some defects with optical transitions in the telecom range have been identified, allowing to interface with fiber networks without the need for wavelength conversion. These unique properties make SiC an attractive platform for the implementation of quantum nodes for quantum communication networks. We provide an overview of the most prominent defects in SiC and their implementation in spin-photon interfaces. Furthermore, we model an exemplary, memory-enhanced quantum communication protocol in order to extract the parameters required to surpass a direct point-to-point link performance. Based on these insights, we summarize the key steps required towards the deployment of SiC devices in large-scale quantum communication networks.

quant-ph↗
arXiv2023

Charge dynamics in the 2D/3D semiconductor heterostructure WSe$_2$/GaAs

Understanding the relaxation and recombination processes of excited states in two-dimensional (2D)/three-dimensional (3D) semiconductor heterojunctions is essential for developing efficient optical and (opto)electronic devices which integrate new 2D materials with more conventional 3D ones. In this work, we unveil the carrier dynamics and charge transfer in a monolayer of WSe$_2$ on a GaAs substrate. We use time-resolved differential reflectivity to study the charge relaxation processes involved in the junction and how they change when compared to an electrically decoupled heterostructure, WSe$_2$/hBN/GaAs. We observe that the monolayer in direct contact with the GaAs substrate presents longer optically-excited carrier lifetimes (3.5 ns) when compared with the hBN-isolated region (1 ns), consistent with a strong reduction of radiative decay and a fast charge transfer of a single polarity. Through low-temperature measurements, we find evidence of a type-II band alignment for this heterostructure with an exciton dissociation that accumulates electrons in the GaAs and holes in the WSe$_2$. The type-II band alignment and fast photo-excited carrier dissociation shown here indicate that WSe$_2$/GaAs is a promising junction for new photovoltaic and other optoelectronic devices, making use of the best properties of new (2D) and conventional (3D) semiconductors.

cond-mat.mes-hall↗
arXiv2023

Magnetic field control of light-induced spin accumulation in monolayer MoSe$_2$

Semiconductor transition metal dichalcogenides (TMDs) have equivalent dynamics for their two spin/valley species. This arises from their energy-degenerated spin states, connected via time-reversal symmetry. When an out-of-plane magnetic field is applied, time-reversal symmetry is broken and the energies of the spin-polarized bands shift, resulting in different bandgaps and dynamics in the K$_+$ and K$_-$ valleys. Here, we use time-resolved Kerr rotation to study the magnetic field dependence of the spin dynamics in monolayer MoSe$_2$. We show that the magnetic field can control the light-induced spin accumulation of the two valley states, with a small effect on the recombination lifetimes. We unveil that the magnetic field-dependent spin accumulation is in agreement with hole spin dynamics at the longer timescales, indicating that the electron spins have faster relaxation rates. We propose a rate equation model that suggests that lifting the energy-degeneracy of the valleys induces an ultrafast spin-flip toward the stabilization of the valley with the higher valence band energy. Our results provide an experimental insight into the ultrafast charge and spin dynamics in TMDs and a way to control it, which will be useful for the development of new spintronic and valleytronic applications.

cond-mat.mes-hall↗
arXiv2022

Coherent spin dynamics of hyperfine-coupled vanadium impurities in silicon carbide

Progress with quantum technology has for a large part been realized with the nitrogen-vacancy centre in diamond. Part of its properties, however, are nonideal and this drives research into other spin-active crystal defects. Several of these come with much stronger energy scales for spin-orbit and hyperfine coupling, but how this affects their spin coherence is little explored. Vanadium in silicon carbide is such a system, with technological interest for its optical emission at a telecom wavelength and compatibility with semiconductor industry. Here we show coherent spin dynamics of an ensemble of vanadium defects around a clock-transition, studied while isolated from, or coupled to neighbouring nuclear spins. We find spin dephasing times up to 7.2 $μ$s, and via spin-echo studies coherence lifetimes that go well beyond tens of microseconds. We demonstrate operation points where strong coupling to neighbouring nuclear spins does not compromise the coherence of the central vanadium spin, which identifies how these can be applied as a coherent spin register. Our findings are relevant for understanding a wide class of defects with similar energy scales and crystal symmetries, that are currently explored in diamond, silicon carbide, and hexagonal boron nitride.

quant-ph↗
arXiv2022

Electromagnetically induced transparency in inhomogeneously broadened divacancy defect ensembles in SiC

Electromagnetically induced transparency (EIT) is a phenomenon that can provide strong and robust interfacing between optical signals and quantum coherence of electronic spins. In its archetypical form, mainly explored with atomic media, it uses a (near-)homogeneous ensemble of three-level systems, in which two low-energy spin-1/2 levels are coupled to a common optically excited state. We investigate the implementation of EIT with c-axis divacancy color centers in silicon carbide. While this material has attractive properties for quantum device technologies with near-IR optics, implementing EIT is complicated by the inhomogeneous broadening of the optical transitions throughout the ensemble and the presence of multiple ground-state levels. These may lead to darkening of the ensemble upon resonant optical excitation. Here, we show that EIT can be established with high visibility also in this material platform upon careful design of the measurement geometry. Comparison of our experimental results with a model based on the Lindblad equations indicates that we can create coherences between different sets of two levels all-optically in these systems, with potential impact for RF-free quantum sensing applications. Our work provides an understanding of EIT in multi-level systems with significant inhomogeneities, and our considerations are valid for a wide array of defects in semiconductors.

quant-ph↗
arXiv2022

Broadband single-mode planar waveguides in monolithic 4H-SiC

Color-center defects in silicon carbide promise opto-electronic quantum applications in several fields, such as computing, sensing and communication. In order to scale down and combine these functionalities with the existing silicon device platforms, it is crucial to consider SiC integrated optics. In recent years many examples of SiC photonic platforms have been shown, like photonic crystal cavities, film-on-insulator waveguides and micro-ring resonators. However, all these examples rely on separating thin films of SiC from substrate wafers. This introduces significant surface roughness, strain and defects in the material, which greatly affects the homogeneity of the optical properties of color centers. Here we present and test a method for fabricating monolithic single-crystal integrated-photonic devices in SiC: tuning optical properties via charge carrier concentration. We fabricated monolithic SiC n-i-n and p-i-n junctions where the intrinsic layer acts as waveguide core, and demonstrate the waveguide functionality for these samples. The propagation losses are below 14 dB/cm. These waveguide types allow for addressing color-centers over a broad wavelength range with low strain-induced inhomogeneity of the optical-transition frequencies. Furthermore, we expect that our findings open the road to fabricating waveguides and devices based on p-i-n junctions, which will allow for integrated electrostatic and radio frequency (RF) control together with high-intensity optical control of defects in silicon carbide.

physics.optics↗
arXiv2021

Hyperfine-mediated transitions between electronic spin-1/2 levels of transition metal defects in SiC

Transition metal defects in SiC give rise to localized electronic states that can be optically addressed in the telecom range in an industrially mature semiconductor platform. This has led to intense scrutiny of the spin and optical properties of these defect centers. For spin-1/2 defects, a combination of the defect symmetry and the strong spin-orbit coupling may restrict the allowed spin transitions, giving rise to defect spins that are long lived, but hard to address via microwave spin manipulation. Here, we show via analytical and numerical results that the presence of a central nuclear spin can lead to a non-trivial mixing of electronic spin states, while preserving the defect symmetry. The interplay between a small applied magnetic field and hyperfine coupling opens up magnetic microwave transitions that are forbidden in the absence of hyperfine coupling, enabling efficient manipulation of the electronic spin. We also find that an electric microwave field parallel to the c-axis can be used to manipulate the electronic spin via modulation of the relative strength of the dipolar hyperfine term.

quant-ph↗
arXiv2021

Symmetry and Control of Spin-Scattering Processes in Two-Dimensional Transition Metal Dichalcogenides

Transition metal dichalcogenides (TMDs) combine interesting optical and spintronic properties in an atomically-thin material, where the light polarization can be used to control the spin and valley degrees-of-freedom for the development of novel opto-spintronic devices. These promising properties emerge due to their large spin-orbit coupling in combination with their crystal symmetries. Here, we provide simple symmetry arguments in a group-theory approach to unveil the symmetry-allowed spin scattering mechanisms, and indicate how one can use these concepts towards an external control of the spin lifetime. We perform this analysis for both monolayer (inversion asymmetric) and bilayer (inversion symmetric) crystals, indicating the different mechanisms that play a role in these systems. We show that, in monolayer TMDs, electrons and holes transform fundamentally differently -- leading to distinct spin-scattering processes. We find that one of the electronic states in the conduction band is partially protected by time-reversal symmetry, indicating a longer spin lifetime for that state. In bilayer and bulk TMDs, a hidden spin-polarization can exist within each layer despite the presence of global inversion symmetry. We show that this feature enables control of the interlayer spin-flipping scattering processes via an out-of-plane electric field, providing a mechanism for electrical control of the spin lifetime.

cond-mat.mes-hall↗
arXiv2020

The role of device asymmetries and Schottky barriers on the helicity-dependent photoresponse of 2D phototransistors

Circular photocurrents (CPC), namely circular photogalvanic (CPGE) and photon drag effects, have recently been reported both in monolayer and multilayer transition metal dichalcogenide (TMD) phototransistors. However, the underlying physics for the emergence of these effects are not yet fully understood. In particular, the emergence of CPGE is not compatible with the D3h crystal symmetry of two-dimensional TMDs, and should only be possible if the symmetry of the electronic states is reduced by influences such as an external electric field or mechanical strain. Schottky contacts, nearly ubiquitous in TMD-based transistors, can provide the high electric fields causing a symmetry breaking in the devices. Here, we investigate the effect of these Schottky contacts on the CPC by characterizing the helicity-dependent photoresponse of monolayer MoSe2 devices both with direct metal-MoSe2 Schottky contacts and with h-BN tunnel barriers at the contacts. We find that, when Schottky barriers are present in the device, additional contributions to CPC become allowed, resulting in emergence of CPC for illumination at normal incidence.

cond-mat.mtrl-sci↗
arXiv2020

Detecting chirality in two-terminal electronic devices

Central to spintronics is the interconversion between electronic charge and spin currents, and this can arise from the chirality-induced spin selectivity (CISS) effect. CISS is often studied as magnetoresistance (MR) in two-terminal (2T) electronic devices containing a chiral (molecular) component and a ferromagnet. However, fundamental understanding of when and how this MR can occur is lacking. Here, we uncover an elementary mechanism that generates such a MR for nonlinear response. It requires energy-dependent transport and energy relaxation within the device. The sign of the MR depends on chirality, charge carrier type, and bias direction. Additionally, we reveal how CISS can be detected in the linear response regime in magnet-free 2T devices, either by forming a chirality-based spin-valve using two or more chiral components, or by Hanle spin precession in devices with a single chiral component. Our results provide operation principles and design guidelines for chirality-based spintronic devices and technologies.

cond-mat.mes-hall↗
arXiv2019

Spin-relaxation times exceeding seconds for color centers with strong spin-orbit coupling in SiC

Spin-active color centers in solids show good performance for quantum technologies. Several transition-metal defects in SiC offer compatibility with telecom and semiconductor industries. However, whether their strong spin-orbit coupling degrades their spin lifetimes is not clear. We show that a combination of a crystal-field with axial symmetry and spin-orbit coupling leads to a suppression of spin-lattice and spin-spin interactions, resulting in remarkably slow spin relaxation. Our optical measurements on an ensemble of Mo impurities in SiC show a spin lifetime $T_1$ of $2,4$ s at $2$ K.

quant-ph↗
arXiv2019

Circuit-Model Analysis for Spintronic Devices with Chiral Molecules as Spin Injectors

Recent research discovered that charge transfer processes in chiral molecules can be spin selective and named the effect chiral-induced spin selectivity (CISS). Follow-up work studied hybrid spintronic devices with conventional electronic materials and chiral (bio)molecules. However, a theoretical foundation for the CISS effect is still in development and the spintronic signals were not evaluated quantitatively. We present a circuit-model approach that can provide quantitative evaluations. Our analysis assumes the scheme of a recent experiment that used photosystem~I (PSI) as spin injectors, for which we find that the experimentally observed signals are, under any reasonable assumptions on relevant PSI time scales, too high to be fully due to the CISS effect. We also show that the CISS effect can in principle be detected using the same type of solid-state device, and by replacing silver with graphene, the signals due to spin generation can be enlarged four orders of magnitude. Our approach thus provides a generic framework for analyzing this type of experiments and advancing the understanding of the CISS effect.

cond-mat.mes-hall↗
arXiv2019

Semiconductor channel mediated photodoping in h-BN encapsulated monolayer MoSe2 phototransistors

In optically excited two-dimensional phototransistors, charge transport is often affected by photodoping effects. Recently, it was shown that such effects are especially strong and persistent for graphene/h-BN heterostructures, and that they can be used to controllably tune the charge neutrality point of graphene. In this work we investigate how this technique can be extended to h BN encapsulated monolayer MoSe_2 phototransistors at room temperature. By exposing the sample to 785 nm laser excitation we can controllably increase the charge carrier density of the MoSe_2 channel by Δn {\approx} 4.45 {\times} 10^{12} cm^{-2}, equivalent to applying a back gate voltage of 60 V. We also evaluate the efficiency of photodoping at different illumination wavelengths, finding that it is strongly correlated with the light absorption by the MoSe_2 layer, and maximizes for excitation on-resonance with the A exciton absorption. This indicates that the photodoping process involves optical absorption by the MoSe_2 channel, in contrast with the mechanism earlier described for graphene/h-BN heterostroctures.

physics.app-ph↗
arXiv2019

Spin-Dependent Electron Transmission Model for Chiral Molecules in Mesoscopic Devices

Various device-based experiments have indicated that electron transfer in certain chiral molecules may be spin-dependent, a phenomenon known as the Chiral Induced Spin Selectivity (CISS) effect. However, due to the complexity of these devices and a lack of theoretical understanding, it is not always clear to what extent the chiral character of the molecules actually contributes to the magnetic-field-dependent signals in these experiments. To address this issue, we report here an electron transmission model that evaluates the role of the CISS effect in two-terminal and multi-terminal linear-regime electron transport experiments. Our model reveals that for the CISS effect, the chirality-dependent spin transmission is accompanied by a spin-flip electron reflection process. Furthermore, we show that more than two terminals are required in order to probe the CISS effect in the linear regime. In addition, we propose two types of multi-terminal nonlocal transport measurements that can distinguish the CISS effect from other magnetic-field-dependent signals. Our model provides an effective tool to review and design CISS-related transport experiments, and to enlighten the mechanism of the CISS effect itself.

cond-mat.mes-hall↗
arXiv2018

Identification and tunable optical coherent control of transition-metal spins in silicon carbide

Color centers in wide-bandgap semiconductors are attractive systems for quantum technologies since they can combine long-coherent electronic spin and bright optical properties. Several suitable centers have been identified, most famously the nitrogen-vacancy defect in diamond. However, integration in communication technology is hindered by the fact that their optical transitions lie outside telecom wavelength bands. Several transition-metal impurities in silicon carbide do emit at and near telecom wavelengths, but knowledge about their spin and optical properties is incomplete. We present all-optical identification and coherent control of molybdenum-impurity spins in silicon carbide with transitions at near-infrared wavelengths. Our results identify spin $S=1/2$ for both the electronic ground and excited state, with highly anisotropic spin properties that we apply for implementing optical control of ground-state spin coherence. Our results show optical lifetimes of $\sim$60 ns and inhomogeneous spin dephasing times of $\sim$0.3 $μ$s, establishing relevance for quantum spin-photon interfacing.

cond-mat.mtrl-sci↗
arXiv2018

Symmetry regimes for circular photocurrents in monolayer MoSe2

In monolayer transition metal dichalcogenides helicity-dependent charge and spin photocurrents can emerge, even without applying any electrical bias, due to circular photogalvanic and photon drag effects. Exploiting such circular photocurrents (CPC) in devices, however, requires better understanding of their behavior and physical origin. Here, we present symmetry, spectral, and electrical characteristics of CPC from excitonic interband transitions in a MoSe2 monolayer. The dependence on bias and gate voltages reveals two different CPC contributions, dominant at different voltages and with different dependence on illumination wavelength and incidence angles. We theoretically analyze symmetry requirements for effects that can yield CPC and compare these with the observed angular dependence and symmetries that occur for our device geometry. This reveals that the observed CPC effects require a reduced device symmetry, and that effects due to Berry curvature of the electronic states do not give a significant contribution.

cond-mat.mtrl-sci↗
arXiv2017

Observation of bright and dark exciton transitions in monolayer MoSe2 by photocurrent spectroscopy

We investigate the excitonic transitions in single- and few-layer MoSe2 phototransistors by photocurrent spectroscopy. The measured spectral profiles show a well-defined peak at the optically active (bright) A0 exciton resonance. More interestingly, when a gate voltage is applied to the MoSe2 to bring its Fermi level near the bottom of the conduction band, another prominent peak emerges at an energy 30 meV above the A0 exciton. We attribute this second peak to a gate-induced activation of the spin-forbidden dark exciton transition, AD0. Additionally, we evaluate the thickness-dependent optical bandgap of the fabricated MoSe2 crystals by characterizing their absorption edge.

cond-mat.mtrl-sci↗