Second-Harmonic Generation in Bulk Diamond Based on Inversion Symmetry Breaking by Color Centers

Abstract

Breaking inversion symmetry in solids plays a central role in nonlinear optics because it can change material properties, such as producing even-order nonlinear optical (NLO) effects. Although a centrosymmetric diamond has been developed as a photonic platform, including waveguides and light sources, the NLO effects in bulk diamonds are limited to the third-order. Thus, exploiting more powerful second-order NLO effects, such as second harmonic generation (SHG), are still challenging. Here we explore symmetry-breaking-induced second-order NLO effects in bulk diamonds using the color center, nitrogen-vacancy center. Exciting with ultrashort laser pulses, SHG and third-harmonic generation (THG) are simultaneously observed at the same time, exhibiting characteristic intensity patterns, depending on both the excitation fluence and the angle of light polarization. We uncovered that SHG serves as the source for THG by the cascading process. Our findings will offer NLO effect-based quantum sensing by diamond color centers, such as imaging of the electromagnetic field by electro-optic effects on the nanofemto scale.

arXiv comment13 pages, 4 figures

References in corpus (12)

• Observation of Intense Second Harmonic Generation from MoS${}_2$ Atomic Crystals
• Atomic-scale imaging of a 27-nuclear-spin cluster using a single-spin quantum sensor
• Scanned probe imaging of nanoscale magnetism at cryogenic temperatures with a single-spin quantum sensor
• Phonon networks with SiV centers in diamond waveguides
• Continuous-wave room-temperature diamond maser
• Optical holonomic single quantum gates with a geometric spin under a zero field
• Nonlinear optical probe of tunable surface electrons on a topological insulator
• Cavity quantum electrodynamics with color centers in diamond
• Terahertz sum-frequency excitation of a Raman-active phonon
• Nonlinear optical spectrum of diamond at femtosecond regime
• Giant nonlinear optical effects induced by nitrogen-vacancy centers in diamond crystals
• Coupling a single NV center with a superconducting qubit via the electro-optic effect

Cited by in corpus (9)

• Temperature-dependent second-harmonic generation from color centers in diamond
• Highly-efficient third-harmonic generation from ultrapure diamond crystals
• Localized Nitrogen-Vacancy centers generated by low-repetition rate fs-laser pulses
• Ultrafast opto-magnetic effects induced by nitrogen-vacancy centers in diamond crystals
• Cooperative dynamic polaronic picture of diamond color centers
• Optical Switching of ${\chi }^{(2)}$ in Diamond Photonics
• An ultrafast diamond nonlinear photonic sensor
• Scalable Reshaping of Diamond Particles via Programmable Nanosculpting
• Plasmon-enhanced ultrafast time-resolved spectroscopy of NV-containing diamond