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The Zeeman splitting and degree of circular polarization (DCP) of photoluminescence (PL) from type-II submonolayer ZnTe/ZnSe quantum dots (QDs) have been investigated in magnetic fields up to 18 T. To explain the observed relative intensities and energy positions of the σ+ and the σ− PL, a non-Boltzmann distribution for holes with ultra-long spin-flip time, confined to submonolayer QDs, is proposed. The g-factor of electrons, located in the ZnSe barriers, was obtained from fitting the temperature dependence of the DCP, and its value is in excellent agreement with that of bulk ZnSe. The g-factor of type-II excitons was extracted by analyzing the Zeeman splitting, from which the g-factor of holes confined within submonolayer ZnTe QDs was found to be ∼2.65 ± 0.40. This value is considerably larger than that in bulk ZnTe. Tight-binding calculations using an sp3s* model were employed to understand the origin of such an increase. The results of the simulation match the experiment and show that the enhancement of the hole g-factor is mostly caused by a reduced orbital contribution to Zeeman splitting arising from the submonolayer thickness of these QDs. [ABSTRACT FROM AUTHOR]

Linearly polarized photoluminescence is observed for type-II ZnTe/ZnSe submonolayer quantum dots (QDs). The comparison of spectral dependence of the degree of linear polarization (DLP) among four samples indicates that the optical anisotropy is mostly related to the elongation of ZnTe QDs. Numerical calculations based on the occupation probabilities of holes in px and py orbitals are performed to estimate the lateral aspect ratio of the QDs, and it is shown that it varies between 1.1 and 1.4. The value of anisotropic exchange splitting for bright excitonic states is found to be ~200 μeV from the measurement of the degree of circular polarization as a function of the magnetic field. The results also show that heavy-light hole mixing ratio is about 0.16. [ABSTRACT FROM AUTHOR]

Sub-monolayer quantities of Mg are introduced in multilayer stacked ZnMgTe quantum dots (QDs) embedded in ZnSe barriers in order to reduce the hole confinement energy by controlling the bandgaps and band-offsets of ZnTe/ZnSe system having type-II band alignment. The photoluminescence (PL) emission from such ZnMgTe/ZnSe QD structure is found to be a broad band centered at 2.35 eV. The higher energy side of the PL band shows a larger blue-shift with increasing excitation intensity and a faster life-time decay due to a greater contribution of the emission from the smaller size dots and the isoelectronic bound excitons. It is found that the characteristic decay time of the PL evolves along the band with a value of 129 ns at 2.18 eV to 19 ns at 2.53 eV. The temperature dependent PL emission is controlled by two thermally activated processes: ionization of electrons away from QD state to the barrier (EA1 ∼ 3 meV) by breaking the type-II excitons and thermal escape of the holes from the ground state to the barrier (EA2 ∼ 114-116 meV). We propose a modified band diagram and energy levels for this ZnMgTe/ZnSe multilayer QD system by determining the composition of Mg inside the QDs and solving the 1-D Schrodinger's equation and show that Mg incorporation lowers the hole activation energy via modification of the valence band offset without changing the barrier significantly. [ABSTRACT FROM AUTHOR]

Abstract: Intermediate band solar cells can potentially have an efficiency of ~63% under full solar concentration, but the material systems investigated until now are far from optimum and are fraught with growth related issues such as low quantum dot densities, presence of wetting layers, and strain driven dislocations. Also, incorporation of type-I quantum dots increases carrier recombination rates, resulting in inferior performance. Here, we show that a novel material system with stacked type-II ZnTe-rich submonolayer QDs embedded in ZnCdSe has close to the optimal material parameters required for an intermediate band material system. We have grown structures comprising of as many as 150 layers of QDs that are formed without wetting layers and that have a valence band offset of ~0.8eV relative to the host with a bandgap of ~2.1eV. We demonstrate the possibility of intermediate band formation and subsequent absorption of below bandgap photons. Additionally, these structures are expected to have longer radiative lifetimes and to suppress Auger recombinations owing to their type-II nature. [Copyright &y& Elsevier]

We study the photophysical stability of ensemble near-surface nitrogen vacancy (NV) centers in diamond under vacuum and air. The optically detected magnetic resonance contrast of the NV centers was measured following exposure to laser illumination, showing opposing trends in air compared to vacuum (increasing by up to 9% and dropping by up to 25%, respectively). Characterization using X-ray photoelectron spectroscopy (XPS) suggests a surface reconstruction: In air, atmospheric oxygen adsorption on a surface leads to an increase in NV - fraction, whereas in vacuum, net oxygen desorption increases the NV 0 fraction. NV charge state switching is confirmed by photoluminescence spectroscopy. Deposition of ∼2 nm alumina (Al 2 O 3 ) over the diamond surface was shown to stabilize the NV charge state under illumination in either environment, attributed to a more stable surface electronegativity. The use of an alumina coating on diamond is therefore a promising approach to improve the resilience of NV sensors., Competing Interests: The authors declare no competing financial interest., (© 2024 The Authors. Published by American Chemical Society.)

A broad effort is underway to improve the sensitivity of NMR through the use of dynamic nuclear polarization. Nitrogen vacancy (NV) centers in diamond offer an appealing platform because these paramagnetic defects can be optically polarized efficiently at room temperature. However, work thus far has been mainly limited to single crystals, because most polarization transfer protocols are sensitive to misalignment between the NV and magnetic field axes. Here we study the spin dynamics of NV- 13 C pairs in the simultaneous presence of optical excitation and microwave frequency sweeps at low magnetic fields. We show that a subtle interplay between illumination intensity, frequency sweep rate, and hyperfine coupling strength leads to efficient, sweep-direction-dependent 13 C spin polarization over a broad range of orientations of the magnetic field. In particular, our results strongly suggest that finely tuned, moderately coupled nuclear spins are key to the hyperpolarization process, which makes this mechanism distinct from other known dynamic polarization channels. These findings pave the route to applications where powders are intrinsically advantageous, including the hyperpolarization of target fluids in contact with the diamond surface or the use of hyperpolarized particles as contrast agents for in vivo imaging., Competing Interests: Conflict of interest: Some of the authors have pending patent applications related to the present study: “Orientation-independent, room-temperature, hyperpolarization of diamond nano- and micro-particles,” A.P., A.A., R.N., X. Lv, C.A.M., provisional application US 62/581,238 filed by University of California, Berkeley, November 3, 2017; “Method for hyperpolarizing nuclear spins at arbitrary magnetic fields,” C.A.M., D.P., A. Laraoui, nonprovisional application Serial No. US 14/961,974, filed by Research Foundation-City University of New York (RF-CUNY), December 8, 2015, priority date December 8, 2014, US Patent Publication No. US-2016-0161583-A1 (June 9, 2016); and “Method and apparatus for polarizing nuclear and electronic spins,” C.A.M., nonprovisional application, Serial No. US 14/781,127, International Application No. PCT/US14/33175, filed by Research Foundation-CUNY, April 7, 2014, priority date April 5, 2013, US Patent Publication No. 2016-0054402-A1 (February 25, 2016), International Publication No. WO 2014/165845 A1 (October 9, 2014).

Although the spin properties of superficial shallow nitrogen-vacancy (NV) centers have been the subject of extensive scrutiny, considerably less attention has been devoted to studying the dynamics of NV charge conversion near the diamond surface. Using multicolor confocal microscopy, here we show that near-surface point defects arising from high-density ion implantation dramatically increase the ionization and recombination rates of shallow NVs compared to those in bulk diamond. Further, we find that these rates grow linearly, not quadratically, with laser intensity, indicative of single-photon processes enabled by NV state mixing with other defect states. Accompanying these findings, we observe NV ionization and recombination in the dark, likely the result of charge transfer to neighboring traps. Despite the altered charge dynamics, we show that one can imprint rewritable, long-lasting patterns of charged-initialized, near-surface NVs over large areas, an ability that could be exploited for electrochemical biosensing or to optically store digital data sets with subdiffraction resolution.

Point defects in wide-band-gap semiconductors are emerging as versatile resources for nanoscale sensing and quantum information science, but our understanding of the photoionization dynamics is presently incomplete. Here, we use two-color confocal microscopy to investigate the dynamics of charge in type 1b diamond hosting nitrogen-vacancy (NV) and silicon-vacancy (SiV) centers. By examining the nonlocal fluorescence patterns emerging from local laser excitation, we show that, in the simultaneous presence of photogenerated electrons and holes, SiV (NV) centers selectively transform into the negative (neutral) charge state. Unlike NVs, 532 nm illumination ionizes SiV^{-} via a single-photon process, thus hinting at a comparatively shallower ground state. In particular, slower ionization rates at longer wavelengths suggest the latter lies approximately ∼1.9  eV below the conduction band minimum. Building on the above observations, we demonstrate on-demand SiV and NV charge initialization over large areas via green laser illumination of variable intensity.

The negatively charged nitrogen vacancy (NV - ) center in diamond is the focus of widespread attention for applications ranging from quantum information processing to nanoscale metrology. Although most work so far has focused on the NV - optical and spin properties, control of the charge state promises complementary opportunities. One intriguing possibility is the long-term storage of information, a notion we hereby introduce using NV-rich, type 1b diamond. As a proof of principle, we use multicolor optical microscopy to read, write, and reset arbitrary data sets with two-dimensional (2D) binary bit density comparable to present digital-video-disk (DVD) technology. Leveraging on the singular dynamics of NV - ionization, we encode information on different planes of the diamond crystal with no cross-talk, hence extending the storage capacity to three dimensions. Furthermore, we correlate the center's charge state and the nuclear spin polarization of the nitrogen host and show that the latter is robust to a cycle of NV - ionization and recharge. In combination with super-resolution microscopy techniques, these observations provide a route toward subdiffraction NV charge control, a regime where the storage capacity could exceed present technologies.

The nitrogen-vacancy (NV) centre in diamond is emerging as a promising platform for solid-state quantum information processing and nanoscale metrology. Of interest in these applications is the manipulation of the NV charge, which can be attained by optical excitation. Here, we use two-colour optical microscopy to investigate the dynamics of NV photo-ionization, charge diffusion and trapping in type-1b diamond. We combine fixed-point laser excitation and scanning fluorescence imaging to locally alter the concentration of negatively charged NVs, and to subsequently probe the corresponding redistribution of charge. We uncover the formation of spatial patterns of trapped charge, which we qualitatively reproduce via a model of the interplay between photo-excited carriers and atomic defects. Further, by using the NV as a probe, we map the relative fraction of positively charged nitrogen on localized optical excitation. These observations may prove important to transporting quantum information between NVs or to developing three-dimensional, charge-based memories.