Optical Spin Control Research Articles

Nitrogen-Vacancy Singlet-Manifold Ionization Energy

The singlet states of the negatively charged nitrogen-vacancy centers in diamond play a key role in its optical spin control and readout. In this work, the hitherto unknown ionization energy of the singlet is measured experimentally and found to be in the range 1.91--2.25 eV. This is obtained by analyzing photoluminescence measurements incorporating spin control and nitrogen-vacancy charge state differentiation, along with simulations based on the nitrogen-vacancy's master equation. This work establishes a protocol for a more accurate estimate of this ionization energy, which can possibly lead to improved readout methods.

Layer-dependent optically induced spin polarization in InSe

Optical control of spin in semiconductors has been pioneered using nanostructures of III-V and II-VI semiconductors, but the emergence of two-dimensional van der Waals materials offers an alternative low-dimensional platform for spintronic phenomena. Indium selenide (InSe), a group-III monochalcogenide van der Waals material, has shown promise for opto-electronics due to its high electron mobility, tunable direct bandgap, and quantum transport. There are predictions of spin-dependent optical selection rules suggesting potential for all-optical excitation and control of spin in a two-dimensional layered material. Despite these predictions, layer-dependent optical spin phenomena in InSe have yet to be explored. Here, we present measurements of layer-dependent optical spin dynamics in few-layer and bulk InSe. Polarized photoluminescence reveals layer-dependent optical orientation of spin, thereby demonstrating the optical selection rules in few-layer InSe. Spin dynamics are also studied in many-layer InSe using time-resolved Kerr rotation spectroscopy. By applying out-of-plane and in-plane static magnetic fields for polarized emission measurements and Kerr measurements, respectively, the $g$-factor for InSe was extracted. Further investigations are done by calculating precession values using a $\textbf{k} \cdot \textbf{p}$ model, which is supported by \textit{ab-initio} density functional theory. Comparison of predicted precession rates with experimental measurements highlights the importance of excitonic effects in InSe for understanding spin dynamics. Optical orientation of spin is an important prerequisite for opto-spintronic phenomena and devices, and these first demonstrations of layer-dependent optical excitation of spins in InSe lay the foundation for combining layer-dependent spin properties with advantageous electronic properties found in this material.

Optical control of exciton spin dynamics in layered metal halide perovskites via polaronic state formation

One of the open challenges of spintronics is to control the spin relaxation mechanisms. Layered metal-halide perovskites are an emerging class of semiconductors which possess a soft crystal lattice that strongly couples electronic and vibrational states and show promise for spintronic applications. Here, we investigate the impact of such strong coupling on the spin relaxation of excitons in the layered perovskite BA2FAPbI7 using a combination of cryogenic Faraday rotation and transient absorption spectroscopy. We report an unexpected increase of the spin lifetime by two orders of magnitude at 77 K under photoexcitation with photon energy in excess of the exciton absorption peak, and thus demonstrate optical control over the dominant spin relaxation mechanism. We attribute this control to strong coupling between excitons and optically excited phonons, which form polaronic states with reduced electron-hole wave function overlap that protect the exciton spin memory. Our insights highlight the special role of exciton-lattice interactions on the spin physics in the layered perovskites and provide a novel opportunity for optical spin control.

Two-qubit logic gates based on the ultrafast spin transfer in π-conjugated graphene nanoflakes

Ultrafast optical spin control allows gate operations to be performed within picosecond time scale, orders of magnitude faster than microwave or electrical control. Here, using high-level quantum chemical computations, we suggest several two-qubit logic gates based on the optically induced ultrafast spin-flip and spin-transfer processes on rhombic graphene nanoflakes (Co4-GNF). It is demonstrated that Co atoms chemisorbed on π-conjugated C atoms can significantly influence the spin properties of the system. The spin density of different energy levels is distributed on different Co atoms, thus opening channels for successful spin-transfer processes between the Co atoms. Reversible local spin-flip processes on each Co atom as well as global spin-transfer processes between the Co atoms are realized. By carefully combining the various spin-dynamics processes achieved in our Co4-GNF structure, both classical (OR, AND, NAND) and quantum (CNOT, SWAP) binary logic gates are constructed. All spin manipulation processes finish at the subpicosecond time scale with fidelities above 96%. This theoretical design, which is exclusively based on laser-induced ultrafast spin dynamics, represents a novel implementation of qubit manipulation and can thus pave the way towards the construction of nano magnetic logic circuits and spintronic devices.

Optical spin control and coherence properties of acceptor bound holes in strained GaAs

Hole spins in semiconductors are a potential qubit alternative to electron spins. In nuclear-spin-rich host crystals like GaAs, the hyperfine interaction of hole spins with nuclei is considerably weaker than that for electrons, leading to potentially longer coherence times. Here we demonstrate optical pumping and coherent population trapping for acceptor-bound holes in a strained GaAs epitaxial layer. We find $\mu$s-scale longitudinal spin relaxation time T$_1$ and an inhomogeneous dephasing time T$_2^*$ of $\sim$7~ns. We attribute the spin relaxation mechanism to a combination effect of a hole-phonon interaction through the deformation potentials and a heavy-hole light-hole mixing in an in-plane magnetic field. We attribute the short T$_2^*$ to g-factor broadening due to strain inhomogeneity. T$_1$ and T$_2^*$ are quantitatively calculated based on these mechanisms and compared with the experimental results. While the hyperfine-mediated decoherence is mitigated, our results highlight the important contribution of strain to relaxation and dephasing of acceptor-bound hole spins.

Coherent Population Trapping Combined with Cycling Transitions for Quantum Dot Hole Spins Using Triplet Trion States.

Optical spin rotations and cycling transitions for measurement are normally incompatible in quantum dots, presenting a fundamental problem for quantum information applications. Here we show that for a hole spin this problem can be addressed using a trion with one hole in an excited orbital, where strong spin-orbit interaction tilts the spin. Then, a particular trion triplet forms a double Λ system, even in a Faraday magnetic field, which we use to demonstrate fast hole spin initialization and coherent population trapping. The lowest trion transitions still strongly preserve spin, thus combining fast optical spin control with cycling transitions for spin readout.

Coherent Spin-Photon Interface with Waveguide Induced Cycling Transitions.

Solid-state quantum dots are promising candidates for efficient light-matter interfaces connecting internal spin degrees of freedom to the states of emitted photons. However, selection rules prevent the combination of efficient spin control and optical cyclicity in this platform. By utilizing a photonic crystal waveguide we here experimentally demonstrate optical cyclicity up to ≈15 through photonic state engineering while achieving high fidelity spin initialization and coherent optical spin control. These capabilities pave the way towards scalable multiphoton entanglement generation and on-chip spin-photon gates.

Two-Qubit Logic Gates Based on the Ultrafast Spin Transfer in π-Conjugated Graphene Nanoflakes

Ultrafast optical spin control allows gate operations to be performed within a picosecond timescale, orders of magnitude faster than microwave or electrical control. Here, using high-level quantum chemical computations, we suggest a two-qubit logic gate based on the optically induced ultrafast spin-flip and spin-transfer processes over rhombic graphene nanoflakes (Co4-GNF). It is demonstrated that the π-conjugated Co atoms can significantly influence the spin properties of the system. The spin density is distributed on different Co atoms in different energy levels, in this way opening a channel for successful spin-transfer processes between the Co atoms. Thus, the reversible local spin-flip processes on each Co atom and global spin-transfer processes between the Co atoms are realized. Importantly, based on various spin-dynamics processes achieved in Co4-GNF structures, both classical (OR, AND, NAND) and quantum (CNOT, SWAP) two-qubit logic gates are constructed, and the spin manipulation process can be completed in subpicosecond timescale with fidelity above 96%. This theoretical design based on the laser-induced ultrafast spin dynamics provides a new implementation of qubit manipulation, which could pave the way towards the construction of nano magnetic logic circuits and spintronic devices.

Optimal quantum optical control of spin in diamond

The nitrogen-vacancy (NV) center spin represents an appealing candidate for quantum information processing. Besides the widely used microwave control, its coherent manipulation may also be achieved using laser as mediated by the excited energy levels. Nevertheless, the multiple levels of the excited state of NV center spin make the coherent transition process become complex and may affect the fidelity of coherent manipulation. Here, we adopt the strategy of optimal quantum control to accelerate coherent state transfer in the ground state manifold of NV center spin using laser. The results demonstrate improved performance in both the speed and the fidelity of coherent state transfer which will be useful for optical control of NV center spin in diamond.

Large g factor in bilayer WS2 flakes

The valley of transition metal dichalcogenides provides an additional platform to manipulate spin due to its unique selection rule. Normally, intralayer optical transitions in the magnetic field show a Zeeman splitting with a g factor of about −4. Here, we report a remarkable valley Zeeman effect exhibited by the splitting of excitonic emission in a bilayer WS2, with a value of g factor as large as −16.5. The observed large g factor results from the interlayer recombination, as the conduction band and the valence band are modified in opposite directions by the magnetic field in different layers. The interlayer recombination is due to the defect induced inversion symmetry breaking, which is theoretically not accessible in ideal bilayer WS2 with inversion symmetry. The large g factor of interlayer emission offers potential benefits for future optical spin control and detection.

Optical Spin Control of Photoexcited Electrons Using a Polarization-controllable Laser

Optical Spin Control of Photoexcited Electrons Using a Polarization-controllable Laser

Advances in Two‐Dimensional Layered Materials

Advances in Two‐Dimensional Layered Materials

Optically switched magnetism in photovoltaic perovskite CH3NH3(Mn:Pb)I3

The demand for ever-increasing density of information storage and speed of manipulation boosts an intense search for new magnetic materials and novel ways of controlling the magnetic bit. Here, we report the synthesis of a ferromagnetic photovoltaic CH3NH3(Mn:Pb)I3 material in which the photo-excited electrons rapidly melt the local magnetic order through the Ruderman–Kittel–Kasuya–Yosida interactions without heating up the spin system. Our finding offers an alternative, very simple and efficient way of optical spin control, and opens an avenue for applications in low-power, light controlling magnetic devices.

Theory of optical spin control in quantum dot microcavities

We present a microscopic theory of optical initialization, control and detection for a single electron spin in a quantum dot embedded into a zero-dimensional microcavity. The strong coupling regime of the trion and the cavity mode is addressed. We demonstrate that efficient spin orientation by a single circularly polarized pulse is possible in relatively weak transverse magnetic fields. The possibilities for spin control by additional circularly polarized pulse are analyzed. Under optimal conditions the Kerr and Faraday rotation angles induced by the spin polarized electron may reach tens of degrees.

Optical control of the spin of a magnetic atom in a semiconductor quantum dot

Abstract:The control of single spins in solids is a key but challenging step for any spin-based solid-state quantumcomputing device. Thanks to their expected long coherence time, localized spins on magnetic atoms in a semiconductor host could be an interesting media to store quantum information in the solid state. Optical probing and control of the spin of individual or pairs of Manganese (Mn) atoms (S = 5/2) have been obtained in II-VI and IIIV semiconductor quantum dots during the last years. In this paper, we review recently developed optical control experiments of the spin of an individual Mn atoms in II-VI semiconductor self-assembled or strain-free quantum dots (QDs).We first show that the fine structure of the Mn atom and especially a strained induced magnetic anisotropy is the main parameter controlling the spin memory of the magnetic atom at zero magnetic field. We then demonstrate that the energy of any spin state of a Mn atom or pairs of Mn atom can be independently tuned by using the optical Stark effect induced by a resonant laser field. The strong coupling with the resonant laser field modifies the Mn fine structure and consequently its dynamics.We then describe the spin dynamics of a Mn atom under this strong resonant optical excitation. In addition to standard optical pumping expected for a resonant excitation, we show that the Mn spin population can be trapped in the state which is resonantly excited. This effect is modeled considering the coherent spin dynamics of the coupled electronic and nuclear spin of the Mn atom optically dressed by a resonant laser field. Finally, we discuss the spin dynamics of a Mn atom in strain-free QDs and show that these structures should permit a fast optical coherent control of an individual Mn spin.

Resonant optical control of the electrically induced spin polarization by periodic excitation

We show that the electron spin polarization generated by an electrical current may have its direction controlled and magnitude amplified by periodic optical excitation. The electrical and optical spin control methods were combined and implemented in a two-dimensional electron gas. By Kerr rotation in an external transverse magnetic field, we demonstrate unexpected long-lived coherent spin oscillations of the current-induced signal in a system with large spin-orbit interaction. Using a single linearly polarized pulse for spin manipulation and detection, we found a strong dependence on the pulse optical power and sample temperature indicating the relevance of the hole spin in the electron spin initialization. The signal was mapped in a Hall bar as function of the position relative to the injection contact. Finally, the presence of an in-plane spin polarization was directly verified by rotating the experimental geometry.

Optically Driven Rabi Oscillations and Adiabatic Passage of Single Electron Spins in Diamond

Rabi oscillations and adiabatic passage of single electron spins in a diamond nitrogen vacancy center are demonstrated with two Raman-resonant optical pulses that are detuned from the respective dipole optical transitions. We show that the optical spin control is nuclear-spin selective and can be robust against rapid decoherence, including radiative decay and spectral diffusion, of the underlying optical transitions. A direct comparison between the Rabi oscillation and the adiabatic passage, along with a detailed theoretical analysis, provides significant physical insights into the connections and differences between these coherent spin processes and also elucidates the role of spectral diffusion in these processes. The optically driven coherent spin processes enable the use of nitrogen vacancy excited states to mediate coherent spin-phonon coupling, opening the door to combining optical control of both spin and mechanical degrees of freedom.

Optical in-plane anisotropy of ZnO/(Zn,Mg)O quantum wells grown ona-plane sapphire: Implications for optical spin control

Utilizing the anisotropic thermal expansion of $a$-plane sapphire, we study the role of anisotropic in-plane strain on ZnO quantum well structures. X-ray data reveal a deformation of the hexagonal unit cell. The symmetry reduction shows up in the optical spectra by distinct linear-polarization features, both for the neutral and charged exciton transition. We elaborate the excitonic fine structure behind this observation, accounting for spin-orbit coupling and electron-hole exchange in the presence of anisotropic strain. The consequences for optical spin control are discussed.

Coherent spin dynamics of donor bound electrons in GaAs

We report experimental studies of coherent spin dynamics of donor-bound electrons in high-purity GaAs by using transient differential transmission. The donor-bound exciton transitions, which are not visible in the linear absorption spectrum, are spectrally resolved in the nonlinear differential transmission spectra. The spin beats in the transient differential transmission response, arising from electron spin precession in an external magnetic field, are investigated with the pump and probe coupling to various donor-bound exciton transitions. The spectral dependence of the spin beats provides important information on the polarization selection rule for the underlying donor-bound exciton transitions. The polarization selection rules deduced from these experiments indicate that contributions from higher-energy donor-bound exciton transitions can severely limit the effectiveness of optical spin control using mechanisms such as polarization-dependent optical Stark shifts.

Quantum control of electron spins in the two-dimensional electron gas of a CdTe quantum well with a pair of Raman-resonant phase-locked laser pulses

We demonstrated optical spin control of a two-dimensional electron gas in a modulation-doped CdTe quantum well by driving a spin-flip Raman transition with a pair of phase-locked laser pulses. In contrast to single-pulse optical spin control, which features a fixed spin-rotation axis, manipulation of the initial relative phase of the pulse pair enables us to control the axis of the optical spin rotation. We show that the Raman pulse pair acts like an effective microwave field, mapping the relative optical phase onto the phase of the electron spin polarization and making possible ultrafast, all-optical, and full quantum control of the electron spins.