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Kipp J. van Schooten

Publications and source records attributed to Kipp J. van Schooten.

7 recordsLinked to original sources

DNP-NMR of surface hydrogen on silicon microparticles

Dynamic nuclear polarization (DNP) enhanced nuclear magnetic resonance (NMR) offers a promising route to studying local atomic environments at the surface of both crystalline and amorphous materials. We take advantage of unpaired electrons due to defects close to the surface of the silicon microparticles to hyperpolarize adjacent $^{1}$H nuclei. At 3.3 T and 4.2 K, we observe the presence of two proton peaks, each with a linewidth on the order of 5 kHz. Echo experiments indicate a homogeneous linewidth of $\sim 150-300$ Hz for both peaks, indicative of a sparse distribution of protons in both environments. The downfield peak at 10 ppm lies within the typical chemical shift range for proton NMR, and was found to be relatively stable over repeated measurements. The upfield peak was found to vary in position between -19 and -37 ppm, well outside the range of typical proton NMR shifts, and indicative of a high-degree of chemical shielding. The upfield peak was also found to vary significantly in intensity across different experimental runs, suggesting a weakly-bound species. These results suggest that the hydrogen is located in two distinct microscopic environments on the surface of these Si particles.

cond-mat.mtrl-sci↗

Optical dependence of electrically-detected magnetic resonance in lightly-doped Si:P devices

Electrically-detected magnetic resonance (EDMR) provides a highly sensitive method for reading out the state of donor spins in silicon. The technique relies on a spin-dependent recombination (SDR) process involving dopant spins that are coupled to interfacial defect spins near the Si/SiO$_2$ interface. To prevent ionization of the donors, the experiments are performed at cryogenic temperatures and the mobile charge carriers needed are generated via optical excitation. The influence of this optical excitation on the SDR process and the resulting EDMR signal is still not well understood. Here, we use EDMR to characterize changes to both phosphorus and defect spin readout as a function of optical excitation using: a 980 nm laser with energy just above the silicon band edge at cryogenic temperatures; a 405 nm laser to generate hot surface-carriers; and a broadband white light source. EDMR signals are observed from the phosphorus donor and two distinct defect species in all the experiments. With near-infrared excitation, we find that the EDMR signal primarily arises from donor-defect pairs, while at higher photon energies there are significant additional contributions from defect-defect pairs. The optical penetration depth into silicon is also known to be strongly wavelength dependent at cryogenic temperatures. The energy of the optical excitation is observed to strongly modulate the kinetics of the SDR process. Careful tuning of the optical photon energy could therefore be used to control both the subset of spin pairs contributing to the EDMR signal as well as the dynamics of the SDR process.

cond-mat.mes-hall↗

Chemisorption of water on the surface of silicon microparticles measured by DNP-enhanced NMR

We use dynamic nuclear polarization (DNP) enhanced nuclear magnetic resonance (NMR) at liquid helium temperatures to directly detect hydrogen attached to the surface of silicon microparticles. The proton NMR spectrum from a dry sample of polycrystalline silicon powder (1-5 $μ$m) shows a distinctively narrow Lorentzian-shaped resonance with a width of 6.2 kHz, indicative of a very sparse distribution of protons attached to the silicon surface. These protons are within a few atomic monolayers of the silicon surface. The high sensitivity NMR detection of surface protons from low surface area ($0.26 - 1.3 \: m^2/g$) particles is enabled by an overall signal enhancement of 4150 over the room temperature NMR signal at the same field. When the particles were suspended in a solvent with 80% H2O and 20% D2O, the narrow peak was observed to grow in intensity over time, indicating growth of the sparse surface proton layer. However, when the particles were suspended in a solvent with 20% H2O and 80% D2O, the narrow bound-proton peak was observed to shrink due to exchange between the surface protons and the deuterium in solution. This decrease was accompanied by a concomitant growth in the intensity of the frozen solvent peak, as the relative proton concentration of the solvent increased. When the particles were suspended in the organic solvent hexane, the proton NMR spectra remained unchanged over time. These results are consistent with the known chemisorption of water on the silicon surface resulting in the formation of hydride and hydroxyl species. Low-temperature DNP NMR can thus be used as a non-destructive probe of surface corrosion for silicon in aqueous environments. This is important in the context of using silicon MEMS and bioMEMS devices in such environments, for silicon micro- and nano-particle MRI imaging agents, and the use of nanosilicon for splitting water in fuel cells.

cond-mat.mtrl-sci↗

Spintronics Detection of Interfacial Magnetic Switching in a Paramagnetic Tris(8-hydroxyquinoline)iron(III) Thin Film

Organic semiconductors find increasing importance in spin transport devices due to the modulation and control of their properties through chemical synthetic versatility. The organic materials are used as interlayers between two ferromagnet (FM) electrodes in organic spin valves (OSV), as well as for magnetic spin manipulation of metal-organic complexes at the molecular level. In the latter, specifically, the substrate-induced magnetic switching in a paramagnetic molecule has been evoked extensively, but studied by delicate surface spectroscopies. Here we present evidence of the substantial magnetic switching in a nanosized thin film of the paramagnetic molecule, tris(8-hydroxyquinoline)iron(III) (Feq3) deposited on a FM substrate, using the magnetoresistance response of electrical spin-injection in an OSV structure, and the inverse-spin-Hall effect induced by state-of-art pulsed microwave spin-pumping. We show that interfacial spin control at the molecular level may lead to a macroscopic organic spin transport device, thus, bridging the gap between organic spintronics and molecular spintronics.

cond-mat.mtrl-sci↗

Spintronics of Organometal Trihalide Perovskites

The family of organometal trihalide perovskite (OTP), CH3NH3PbX3 (where X is halogen) has recently revolutionized the photovoltaics field and shows promise in a variety of optoelectronic applications. The characteristic spin properties of charge and neutral excitations in OTPs are influenced by the large spin-orbit coupling of the Pb atoms, which may lead to spin-based device applications. Here we report the first studies of pure spin-current and spin-aligned carrier injection in OTP spintronics devices using spin-pumping and spin-injection, respectively. We measure a relatively large inverse-spin-Hall effect using pulsed microwave excitation in OTP devices at resonance with a ferromagnetic substrate, from which we derive room temperature spin diffusion length, lambda_sd~9nm; and low-temperature giant magnetoresistance in OTP-based spin-valves from which we estimate lambda_sd~85nm.

cond-mat.mtrl-sci↗

Inverse Spin Hall Effect from pulsed Spin Current in Organic Semiconductors with Tunable Spin-Orbit Coupling

Exploration of spin-currents in organic semiconductors (OSECs) induced by resonant microwave absorption in ferromagnetic substrates has been of great interest for potential spintronics applications. Due to the inherently weak spin-orbit coupling (SOC) of OSECs, their inverse spin Hall effect (ISHE) response is very subtle; limited by the microwave power applicable under continuous-wave (cw) excitation. Here we introduce a novel approach for generating significant ISHE signals using pulsed ferromagnetic resonance, where the ISHE is ~2-3 orders of magnitude larger compared to cw excitation. This strong ISHE enables us to investigate a variety of OSECs ranging from pi-conjugated polymers with strong SOC that contain intrachain platinum atoms, to weak SOC polymers, to C60 films, where the SOC is predominantly caused by the molecule surface curvature. The pulsed-ISHE technique offers a robust route for efficient injection and detection schemes of spin-currents at room temperature, and paves the way for spin-orbitronics in plastic materials.

cond-mat.mtrl-sci↗

Spin-dependent exciton quenching and intrinsic spin coherence in CdSe/CdS nanocrystals

Large surface to volume ratios of semiconductor nanocrystals cause susceptibility to charge trapping, which can modify luminescence yields and induce single-particle blinking. Optical spectroscopies cannot differentiate between bulk and surface traps in contrast to spin-resonance techniques, which in principle avail chemical information on such trap sites. Magnetic resonance detection via spin-controlled photoluminescence enables the direct observation of interactions between emissive excitons and trapped charges. This approach allows the discrimination of two functionally different trap states in CdSe/CdS nanocrystals underlying the fluorescence quenching and thus blinking mechanisms: a spin-dependent Auger process in charged particles; and a charge-separated state pair process, which leaves the particle neutral. The paramagnetic trap centers offer control of energy transfer from the wide-gap CdS to the narrow-gap CdSe, i.e. light harvesting within the heterostructure. Coherent spin motion within the trap states of the CdS arms of nanocrystal tetrapods is reflected by spatially remote luminescence from CdSe cores with surprisingly long coherence times of >300 ns at 3.5 K.

cond-mat.mes-hall↗