| Summary: | Nitrogen-vacancy centers in diamond have gained widespread attention as quantum systems that can be applied in quantum information devices. The excellent properties of quantum devices can be enhanced using preferentially oriented nitrogen-vacancy (NV) centers. However, thus far, orientation control has been achieved only via chemical vapor deposition. In this study, we demonstrate the creation of preferentially oriented NV centers via laser writing. The alignment ratio of ensemble NV centers is biased along the direction parallel to [111], depending on the femtosecond laser polarization, causing an increase of 55 % in contrast to the optically magnetic resonance signal at maximum compared with 25 % in random orientation. Based on time-dependent density-functional theory (TDDFT) simulations and experimental observations, such complex polarization dependence can be attributed to the anisotropy of electron excitation. This technique provides a new optical fabrication method for engineered materials and devices used in quantum technology.
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