Emma Schmidgall

Layer-dependent ferromagnetism in a van der Waals crystal down to the monolayer limit

Since the discovery of graphene, the family of two-dimensional materials has grown, displaying a broad range of electronic properties. Recent additions include semiconductors with spin–valley coupling, Ising superconductors that can be tuned into a quantum metal, possible Mott insulators with tunable charge-density waves, and topological semimetals with edge transport. However, no two-dimensional crystal with intrinsic magnetism has yet been discovered; such a crystal would be useful in many technologies from sensing to data storage. Theoretically, magnetic order is prohibited in the two-dimensional isotropic Heisenberg model at finite temperatures by the Mermin–Wagner theorem. Magnetic anisotropy removes this restriction, however, and enables, for instance, the occurrence of two-dimensional Ising ferromagnetism. Here we use magneto-optical Kerr effect microscopy to demonstrate that monolayer chromium triiodide (CrI3) is an Ising ferromagnet with out-of-plane spin orientation. Its Curie temperature of 45 kelvin is only slightly lower than that of the bulk crystal, 61 kelvin, which is consistent with a weak interlayer coupling. Moreover, our studies suggest a layer-dependent magnetic phase, highlighting thickness-dependent physical properties typical of van der Waals crystals. Remarkably, bilayer CrI3 displays suppressed magnetization with a metamagnetic effect, whereas in trilayer CrI3 the interlayer ferromagnetism observed in the bulk crystal is restored. This work creates opportunities for studying magnetism by harnessing the unusual features of atomically thin materials, such as electrical control for realizing magnetoelectronics, and van der Waals engineering to produce interface phenomena.

Graphene-graphite oxide field-effect transistors.

Graphenes high mobility and two-dimensional nature make it an attractive material for field-effect transistors. Previous efforts in this area have used bulk gate dielectric materials such as SiO(2) or HfO(2). In contrast, we have studied the use of an ultrathin layered material, graphenes insulating analogue, graphite oxide. We have fabricated transistors comprising single or bilayer graphene channels, graphite oxide gate insulators, and metal top-gates. The graphite oxide layers show relatively minimal leakage at room temperature. The breakdown electric field of graphite oxide was found to be comparable to SiO(2), typically ~1-3 × 10(8) V/m, while its dielectric constant is slightly higher, κ ≈ 4.3.

Van der Waals engineering of ferromagnetic semiconductor heterostructures for spin and valleytronics

A van der Waals heterostructure of monolayer WSe2 and ferromagnetic CrI3 enables exceptional control of valley pseudospin. The integration of magnetic material with semiconductors has been fertile ground for fundamental science as well as of great practical interest toward the seamless integration of information processing and storage. We create van der Waals heterostructures formed by an ultrathin ferromagnetic semiconductor CrI3 and a monolayer of WSe2. We observe unprecedented control of the spin and valley pseudospin in WSe2, where we detect a large magnetic exchange field of nearly 13 T and rapid switching of the WSe2 valley splitting and polarization via flipping of the CrI3 magnetization. The WSe2 photoluminescence intensity strongly depends on the relative alignment between photoexcited spins in WSe2 and the CrI3 magnetization, because of ultrafast spin-dependent charge hopping across the heterostructure interface. The photoluminescence detection of valley pseudospin provides a simple and sensitive method to probe the intriguing domain dynamics in the ultrathin magnet, as well as the rich spin interactions within the heterostructure.

Deterministic generation of a cluster state of entangled photons

Weaving an entangled cluster Entanglement is a powerful resource for quantum computation and information processing. One requirement is the ability to entangle multiple particles reliably. Schwartz et al. created an on-demand entangled cluster state of several photons by addressing a quantum dot with a sequence of laser pulses (see the Perspective by Briegel). They used an internal state of the quantum dot, a dark exciton, and its association with another internal state, a biexciton, to weave successive photons into an entangled cluster, generating entanglement between up to five photons. Science, this issue p. 434; see also p. 416 A quantum dot is used to realize entangled cluster states of up to five photons. Photonic cluster states are a resource for quantum computation based solely on single-photon measurements. We use semiconductor quantum dots to deterministically generate long strings of polarization-entangled photons in a cluster state by periodic timed excitation of a precessing matter qubit. In each period, an entangled photon is added to the cluster state formed by the matter qubit and the previously emitted photons. In our prototype device, the qubit is the confined dark exciton, and it produces strings of hundreds of photons in which the entanglement persists over five sequential photons. The measured process map characterizing the device has a fidelity of 0.81 with that of an ideal device. Further feasible improvements of this device may reduce the resources needed for optical quantum information processing.

Deterministic Writing and Control of the Dark Exciton Spin Using Single Short Optical Pulses

We experimentally demonstrate deterministic optical writing of a quantum dot-confined dark exciton, in a pure quantum state using one optical pulse. We then control the spin state of this long-lived exciton using picosecond optical pulses.

Efficient Extraction of Zero-Phonon-Line Photons from Single Nitrogen-Vacancy Centers in an Integrated GaP-on-Diamond Platform

Scaling beyond two-node quantum networks using nitrogen vacancy (NV) centers in diamond is limited by the low probability of collecting zero phonon line (ZPL) photons from single centers. Here, we demonstrate GaP-on-diamond disk resonators which resonantly couple ZPL photons from single NV centers to single-mode waveguides. In these devices, the probability of a single NV center emitting a ZPL photon into the guided waveguide mode after optical excitation can reach 9%, due to a combination of resonant enhancement of the ZPL emission and efficient coupling between the resonator and waveguide. We verify the single-photon nature of the emission and experimentally demonstrate both high in-waveguide photon numbers and substantial Purcell enhancement for a set of devices. These devices may enable scalable integrated quantum networks based on NV centers.

Generating single photons at gigahertz modulation-speed using electrically controlled quantum dot microlenses

We report on the generation of single-photon pulse trains at a repetition rate of up to 1 GHz. We achieve this speed by modulating the external voltage applied on an electrically contacted quantum dot microlens, which is optically excited by a continuous-wave laser. By modulating the photoluminescence of the quantum dot microlens using a square-wave voltage, single-photon emission is triggered with a response time as short as (281 ± 19) ps, being 6 times faster than the radiative lifetime of (1.75 ± 0.02) ns. This large reduction in the characteristic emission time is enabled by a rapid capacitive gating of emission from the quantum dot, which is placed in the intrinsic region of a p-i-n-junction biased below the onset of electroluminescence. Here, since our circuit acts as a rectifying differentiator, the rising edge of the applied voltage pulses triggers the emission of single photons from the optically excited quantum dot. The non-classical nature of the photon pulse train generated at GHz-speed is pro...

Optical control of single excitons in semiconductor quantum dots

The fundamental building block of quantum information processing technologies is the quantum-bit a ?qubit.? These technologies require the ability to prepare, control, and read out a qubit state. Spins confined in self-assembled quantum dots are promising candidates for a quantum bit, because semiconductors are compatible with mature modern opto- and micro-electronics. These quantum dot systems offer two more advantages: they are excellent interfaces between the spin state?an anchored qubit and a photon?a ?flying qubit? and they provide means to coherently control the spin qubit by ultrashort optical pulses. In this review, we thoroughly discuss the qubit provided by an optically-excited electron in a quantum dot?the exciton qubit. We demonstrate its spin state initialization, coherent control and read-out using ultrashort optical pulses.

All-optical depletion of dark excitons from a semiconductor quantum dot

Semiconductor quantum dots are considered to be the leading venue for fabricating on-demand sources of single photons. However, the generation of long-lived dark excitons imposes significant limits on the efficiency of these sources. We demonstrate a technique that optically pumps the dark exciton population and converts it to a bright exciton population, using intermediate excited biexciton states. We show experimentally that our method considerably reduces the DE population while doubling the triggered bright exciton emission, approaching thereby near-unit fidelity of quantum dot depletion.

Deterministic generation of a quantum-dot-confined triexciton and its radiative decay via three-photon cascade

Semiconductor quantum dots (QDs) have potential applications in quantum information processing due to the fact that they are potential on-demand sources of single and entangled photons. Generation of polarization-entangled photon pairs was demonstrated using the biexciton-exciton radiative cascade. One obvious way to increase the number of quantum correlated photons that the QDs emit is to use higher-order multiexcitons, in particular the triexciton. Towards achieving this goal, we first demonstrate deterministic generation of the QD-confined triexciton in a well-definedcoherent state and then spectrally identify and directly measure a three-photon radiative cascade resulting from the sequential triexciton-biexciton-exciton radiative recombination.