The ability to control solid-state quantum emitters is fundamental to advancing quantum technologies. The performance of these systems is fundamentally governed by their spin-dependent photodynamics, yet conventional control methods using cavities offer limited access to key non-radiative processes. Here we demonstrate that anisotropic lattice strain serves as a powerful tool for manipulating spin dynamics in solid-state systems. Under high pressure, giant shear strain gradients trigger a complete reversal of the intrinsic spin polarization, redirecting ground-state population from $|0\rangle$ to $|\pm 1\rangle$ manifold. We show that this reprogramming arises from strain-induced mixing of the NV center's excited states and dramatic alteration of intersystem crossing, which we quantify through a combination of opto-magnetic spectroscopy and a theoretical model that disentangles symmetry-preserving and symmetry-breaking strain contributions. Furthermore, the polarization reversal is spatially mapped with a transition region below 120 nm, illustrating sub-diffraction-limit control. Our work establishes strain engineering as a powerful tool for tailoring quantum emitter properties, opening avenues for programmable quantum light sources, high-density spin-based memory, and hybrid quantum photonic devices.
The ability to control solid-state quantum emitters is fundamental to advancing quantum technologies. The performance of these systems is fundamentally governed by their spin-dependent photodynamics, yet conventional control methods using cavities offer limited access to key non-radiative processes. Here we demonstrate that anisotropic lattice strain serves as a powerful tool for manipulating spin dynamics in solid-state systems. Under high pressure, giant shear strain gradients trigger a complete reversal of the intrinsic spin polarization, redirecting ground-state population from ∣0⟩ to ∣±1⟩ manifold. We show that this reprogramming arises from strain-induced mixing of the NV center's excited states and dramatic alteration of intersystem crossing, which we quantify through a combination of opto-magnetic spectroscopy and a theoretical model that disentangles symmetry-preserving and symmetry-breaking strain contributions. Furthermore, the polarization reversal is spatially mapped with a transition region below 120 nm, illustrating sub-diffraction-limit control. Our work establishes strain engineering as a powerful tool for tailoring quantum emitter properties, opening avenues for programmable quantum light sources, high-density spin-based memory, and hybrid quantum photonic devices.
The ability to control solid-state quantum emitters is fundamental to advancing quantum technologies. The performance of these systems is fundamentally governed by their spin-dependent photodynamics, yet conventional control methods using cavities offer limited access to key nonradiative processes. Here we demonstrate that anisotropic lattice strain serves as a powerful tool for manipulating spin dynamics in solid-state systems. Under high pressure, giant shear strain gradients trigger a complete reversal of the intrinsic spin polarization, redirecting ground-state population from |0⟩ to |±1⟩ manifold. We show that this reprogramming arises from strain-induced mixing of the NV center's excited states and dramatic alteration of intersystem crossing, which we quantify through a combination of optomagnetic spectroscopy and a theoretical model that disentangles symmetry-preserving and symmetry-breaking strain contributions. Furthermore, the polarization reversal is spatially mapped with a transition region below 120 nm, illustrating sub-diffraction-limit control. Our Letter establishes strain engineering as a powerful tool for tailoring quantum emitter properties, opening avenues for programmable quantum light sources, high-density spin-based memory, and hybrid quantum photonic devices.
Strain engineering is vital for tuning the optical and spin properties of solid-state color centers, enhancing spin coherence and compensating emission wavelength shift. Here, we develop an all-optical approach to directly modify the local strain of color centers at the nanoscale by migrating the nearby defect. High-power pulsed optical irradiation triggers defect migration, which subsequently leads to the redistribution of the local crystal lattice of the host material. This redistribution alters the strain experienced by nearby color centers. Using silicon-vacancy centers in diamond, we validate this method and demonstrate a ground state splitting enhancement of up to 1.8 THz. Unlike conventional methods, our approach requires no external fields or nanostructure modifications, enabling non-volatile strain control and optical memory functionality across wide temperature ranges. Its local, permanent nature offers a scalable path for enhancing spin coherence in large-scale quantum systems and has potential applications in photonic machine learning. Strain engineering can be used to control spin and optical properties of defect centers. Xue et al. report an all-optical method to reconfigure and increase the local strain of color centers in diamond, which, unlike previous approaches, does not require external fields or nanostructure modifications.
Electron and nuclear spins of diamond nitrogen-vacancy (NV) centers are good candidates for quantum information processing as they have long coherence time and can be initialized and read out optically. However, creating a large number of coherently coupled and individually addressable NV centers for quantum computing has been a big challenge. Here we propose methods to use high-density diamond NV centers coupled by spin-spin interaction with an average separation on the order of 10 nm for quantum computing. We propose to use a strain gradient to encode the position information of each NV center in the energy level of its excited electron orbital state, which causes a shift of its optical transition frequency. With such strain encoding, more than 100 closely-packed NV centers below optical diffraction limit can be read out individually by resonant optical excitation. A magnetic gradient will be used to shift the electron spin resonant (ESR) frequencies of NV centers. Therefore, the spin state of each NV center can be individually manipulated and different NV centers can be selectively coupled. A universal set of quantum operations for two-qubit and three-qubit system is introduced by careful design of external drives. Moreover, entangled states with multiple qubits can be created by this protocol, which is a major step towards quantum information processing with solid-state spins.
Silicon vacancy (VSi) centers in 4H silicon carbide have emerged as a highly promising platform for semiconductor-based quantum technologies, combining excellent spin and optical properties with an industrial-grade, CMOS-compatible material. As these defects are increasingly integrated into practical quantum devices, they inevitably encounter lattice strain. However, while the impact of strain is well documented for other solid-state defects like NV centers in diamond, its specific influence on key VSi spin dynamics such as initialization fidelity and state lifetimes remain largely unexplored. In this work, we address this critical gap by designing fully optical pulse sequences and incorporating the effective spin-3/2 strain Hamiltonian into our analysis. This combined approach allows us to isolate both axial and transverse strain contributions and systematically characterize their effect on the metastable state transition rates. Specifically, we reveal that strain significantly reduces the transition rates from the energetically lowest metastable state to the ground state quartet, leading to decreased photon emission. Supported by first-principles calculations, our findings provide a deeper understanding of VSi spin-strain dynamics, yielding crucial insights for the robust deployment of these centers in realistic, strain-prone environments.
The nitrogen-vacancy (NV) center in diamond has garnered great interest over the past decade as its electronic spin shows promise as a quantum bit (qubit) and nanoscale sensor. Consisting of a substitutional nitrogen adjacent to a vacant site within the carbon lattice of diamond, this defect exhibits millisecond-long spin coherence times extending beyond room temperature, spin-dependent optical addressability, coupling to intrinsic and nearby nuclear spins, and it can be controlled and manipulated through electrical, magnetic, and optical means. In particular, at cryogenic temperatures (T < 25 K), the NV center's excited state becomes sharp and optically resolvable, providing a solid-state quantum optical testbed. In this thesis, I describe several experiments that explore this quantum optical interface to facilitate the development of a photonic network of single spins linked and controlled by light. We begin by exploring how electric fields tune the orbital levels within the NV center through the DC Stark effect, finding a surprising photo-induced field that aids in the ability to tune multiple NV centers' optical transitions to degeneracy. We then develop techniques to fully control the spin state of the NV center by coupling through a lambda system, an energy configuration consisting of two lower levels coupled to one of higher energy. When a lambda system is optically driven, the spin becomes trapped in a dark state, or the eigenstate of the system that is not coupled to the light fields through destructive interference, forming the basis for the various types of control demonstrated. We demonstrate arbitrary-basis initialization and readout of the spin state through coherent population trapping, as well as the ability to rotate about any arbitrary basis through stimulated Raman transitions. Combining these techniques, we measure the NV center's spin coherence through a completely optical measurement. We then extend these lambda system techniques to adiabatically move the dark state in trajectories around the Bloch sphere. Such trajectories accumulate a quantum mechanical phase that depends only on the geometry of the path enclosed, not on the energetics or time of the interaction. We characterize the interaction, measure this phase, known as Berry phase, and explore the limits of its control and resilience to noise. Finally, we demonstrate another all-optical control technique that uses strong ultrafast pulses of light to transfer the spin between the ground and excited states, deriving spin manipulation from the excited state dynamics. This technique also provides time-resolved spectroscopy of the excited state and its various decay and decoherence mechanisms. These experiments advance the progress toward the development of photonic networks coupling and controlling defects through light-matter interactions.
The study of individual quantum systems in solids, for use as quantum bits (qubits) and probes of decoherence, requires protocols for their initialization, unitary manipulation, and readout. In many solid-state quantum systems, these operations rely on disparate techniques that can vary widely depending on the particular qubit structure. One such qubit, the nitrogen-vacancy (NV) center spin in diamond, can be initialized and read out through its special spin-selective intersystem crossing, while microwave electron spin resonance techniques provide unitary spin rotations. Instead, we demonstrate an alternative, fully optical approach to these control protocols in an NV center that does not rely on its intersystem crossing. By tuning an NV center to an excited-state spin anticrossing at cryogenic temperatures, we use coherent population trapping and stimulated Raman techniques to realize initialization, readout, and unitary manipulation of a single spin. Each of these techniques can be performed directly along any arbitrarily chosen quantum basis, removing the need for extra control steps to map the spin to and from a preferred basis. Combining these protocols, we perform measurements of the NV center's spin coherence, a demonstration of this full optical control. Consisting solely of optical pulses, these techniques enable control within a smaller footprint and within photonic networks. Likewise, this unified approach obviates the need for both electron spin resonance manipulation and spin addressability through the intersystem crossing. This method could therefore be applied to a wide range of potential solid-state qubits, including those which currently lack a means to be addressed.