Thomas Scrace

Magnetoluminescence and valley polarized state of a two-dimensional electron gas in WS2 monolayers.

Materials often exhibit fundamentally new phenomena in reduced dimensions that potentially lead to novel applications. This is true for single-layer, two-dimensional semiconductor crystals of transition-metal dichalcogenides, MX2 (M = Mo, W and X = S, Se). They exhibit direct bandgaps with energies in the visible region at the two non-equivalent valleys in the Brillouin zone. This makes them suitable for optoelectronic applications that range from light-emitting diodes to light harvesting and light sensors, and to valleytronics. Here, we report the results of a magnetoluminescence study of WS2 single-layer crystals in which the strong spin-orbit interaction additionally locks the valley and spin degrees of freedom. The recombination of the negatively charged exciton in the presence of a two-dimensional electron gas (2DEG) is found to be circularly polarized at zero magnetic field despite being excited with unpolarized light, which indicates that the existence of a valley polarized 2DEG is caused by valley and spin locking and strong electron-electron interactions.

Enhanced valley splitting in monolayer WSe2 due to magnetic exchange field

Exploiting the valley degree of freedom to store and manipulate information provides a novel paradigm for future electronics. A monolayer transition-metal dichalcogenide (TMDC) with a broken inversion symmetry possesses two degenerate yet inequivalent valleys, which offers unique opportunities for valley control through the helicity of light. Lifting the valley degeneracy by Zeeman splitting has been demonstrated recently, which may enable valley control by a magnetic field. However, the realized valley splitting is modest (∼0.2 meV T-1). Here we show greatly enhanced valley spitting in monolayer WSe2, utilizing the interfacial magnetic exchange field (MEF) from a ferromagnetic EuS substrate. A valley splitting of 2.5 meV is demonstrated at 1 T by magnetoreflectance measurements and corresponds to an effective exchange field of ∼12 T. Moreover, the splitting follows the magnetization of EuS, a hallmark of the MEF. Utilizing the MEF of a magnetic insulator can induce magnetic order and valley and spin polarization in TMDCs, which may enable valleytronic and quantum-computing applications.

Mn(2+)-Doped CdSe/CdS Core/Multishell Colloidal Quantum Wells Enabling Tunable Carrier-Dopant Exchange Interactions.

In this work, we report the manifestations of carrier-dopant exchange interactions in colloidal Mn(2+)-doped CdSe/CdS core/multishell quantum wells. The carrier-magnetic ion exchange interaction effects are tunable through wave function engineering. In our quantum well heterostructures, manganese was incorporated by growing a Cd0.985Mn0.015S monolayer shell on undoped CdSe nanoplatelets using the colloidal atomic layer deposition technique. Unlike previously synthesized Mn(2+)-doped colloidal nanostructures, the location of the Mn ions was controlled with atomic layer precision in our heterostructures. This is realized by controlling the spatial overlap between the carrier wave functions with the manganese ions by adjusting the location, composition, and number of the CdSe, Cd1-xMnxS, and CdS layers. The photoluminescence quantum yield of our magnetic heterostructures was found to be as high as 20% at room temperature with a narrow photoluminescence bandwidth of ∼22 nm. Our colloidal quantum wells, which exhibit magneto-optical properties analogous to those of epitaxially grown quantum wells, offer new opportunities for solution-processed spin-based semiconductor devices.

Probing the nature of carrier localization in GaInNAs epilayers by optical methods

Photoluminescence (PL), optical pumping, and reflectance studies of nominally undoped and p-type GaInNAs epilayers are presented. The PL peak energy of the nominally undoped sample exhibits an S-shaped dependence on temperature for T < 50 K. This is attributed to recombination of bound excitons localized on traps. The energy of the PL circular-polarization maximum coincides with the energy of the free-exciton related reflectance feature at all temperatures. In heavily p-type samples the S-shaped temperature-dependence of the PL energy disappears, and the PL peak and circular polarization maximum coincide with the reflectance feature at all temperatures, indicating that the PL is free-exciton-like.

Photoluminescence study of Be-acceptors in GaInNAs epilayers

We have studied Be-acceptors in a p-type GaInNAs epilayer using magneto-luminescence spectroscopy. The band edge photoluminescence (PL) spectra at T = 7 K contain two features: the first is associated with the free exciton while the second with the conduction band to acceptor (CB  →  A) transition. The intensity of the latter decreases with increasing temperature while the excitonic feature survives up to T = 250 K. From the energies of the two PL features, as well as the exciton binding energy in GaInNAs, we determined the Be-acceptor binding energy to be equal to 42 meV. The energy of the CB  →  A feature varies linearly with magnetic field B and has a slope of 5.5×10−4 eV/T.

Time resolved photoluminescence study of magnetic CdSe/CdMnS/CdS core/multi-shell nanoplatelets

Colloidal semiconductor nanoplatelets (NPLs) are quasi 2D-nanostructures that are grown and processed inexpensively using a solution based method and thus have recently attracted considerable attention. We observe two features in the photoluminescence spectrum, suggesting two possible recombination channels. Their intensity ratio varies with temperature and two distinct temperature regions are identified; a low temperature region (10K < T < 90K) and a high temperature region (90K < T < 200K). This ratio increases with increasing temperature, suggesting that one recombination channel involves holes that are weakly localized with a localization energy of 0.043meV. A possible origin of these localized states are energy-variations in the xy-plane of the nanoplatelet. The presence of positive photoluminescence circular polarization in the magnetically-doped core/multi-shell NPLs indicates a hole-dopant exchange interaction and therefore the incorporated magnetic Manganese ions act as a marker that determines the location of the localized hole states.1 Time-resolved measurements show two distinct timescales (τfast and τslow) that can be modeled using a rate equation model. We identify these timescales as closely related to the corresponding recombination times for the channels. The stronger hole localization of one of these channels leads to a decreased electron-hole wave function overlap and thus a decreased oscillator strength and an increased lifetime. We show that we can model and understand the magnetic interaction of doped 2D-colloidal nanoplatelets which opens a pathway to solution processable spin controllable light sources.

Magneto-optical studies of CdSe/CdMnS/CdS core/multi-shell colloidal nanoplatelets

We studied the photoluminescence (PL)) from CdSe/CdMnS/CdS core/multi-shell colloidal nanoplatelets, a versatile platform to study the interplay of optical properties and nanomagnetism. The photoluminescence (PL) exhibits σ+ polarization in the applied magnetic field. Our measurement detects the presence of even a single magnetic monolayer shell. The PLL consists of a higher and a lower energy component; the latter exhibits a circular polarization peak. The time-resolved PL (trPL) shows a red shift as function of time delay. At early (later) times the trPL spectra coincide with the high (low) energy PL component. A model is proposed to interpret these results.

Conventional versus unconventional magnetic polarons: ZnMnTe/ZnSe and ZnTe/ZnMnSe quantum dots

We used time resolved photoluminescence (TRPL) spectroscopy to compare the properties of magnetic polarons in two related, spatially indirect, II-VI epitaxially grown quantum dot systems. In sample A (ZnMnTe/ZnSe), the photoexcited holes are confined in the magnetic ZnMnTe quantum dots (QDs), while the electrons remain in the surrounding non-magnetic ZnSe matrix. In sample B (ZnTe/ZnMnSe) on the other hand, the holes are confined in the non-magnetic ZnTe QDs and the electrons move in the magnetic ZnMnSe matrix. The magnetic polaron formation energies, EMP , in these samples were measured from the temporal red-shift of the excitonic emission peak. The magnetic polarons in the two samples exhibit distinct characteristics. In sample A, the magnetic polaron is strongly bound with EMP=35 meV. Furthermore, EMP has unconventionally weak dependence of on both temperature T and magnetic field Bappl . In contrast, magnetic polarons in sample B show conventional characteristics with EMP decreasing with increasing temperature and increasing external magnetic field. We attribute the difference in magnetic polaron properties between the two types of QDs to the difference in the location of the Mn ions in the respective structures.