Optical Absorption and Emission Mechanisms of Single Defects in Hexagonal Boron Nitride
Autor: | N. R. Jungwirth, Gregory D. Fuchs |
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Rok vydání: | 2017 |
Předmět: |
Physics
Quantum Physics Condensed Matter - Materials Science Condensed matter physics Phonon Materials Science (cond-mat.mtrl-sci) FOS: Physical sciences General Physics and Astronomy Hexagonal boron nitride 02 engineering and technology Nitride 021001 nanoscience & nanotechnology Polarization (waves) 01 natural sciences Wavelength Dipole Excited state 0103 physical sciences Quantum Physics (quant-ph) 010306 general physics 0210 nano-technology Excitation |
Zdroj: | Physical review letters. 119(5) |
ISSN: | 1079-7114 |
Popis: | We investigate the polarization selection rules of sharp zero-phonon lines (ZPLs) from isolated defects in hexagonal boron nitride (h-BN) and compare our findings with the predictions of a configuration coordinate model involving two electronic states. Our survey, which spans the spectral range ~550-740 nm, reveals that, in disagreement with a two-level model, the absorption and emission dipoles are often misaligned. We relate the dipole misalignment angle (${\Delta}{\theta}$) to the ZPL Stokes shift (${\Delta}E$) and find that ${\Delta}{\theta}\sim 0{\deg}$ when ${\Delta}E$ corresponds to an allowed h-BN phonon frequency and that $0{\deg}\leq{\Delta}{\theta}\leq 90{\deg}$ when ${\Delta}E$ exceeds the maximum allowed h-BN phonon frequency. Consequently, a two-level configuration coordinate model succeeds at describing excitations mediated by the creation of one optical phonon but fails at describing excitations that require the creation of multiple phonons. We propose that direct excitations requiring the creation of multiple phonons are inefficient due to the low Huang-Rhys factors in h-BN and that these ZPLs are instead excited indirectly via an intermediate electronic state. This hypothesis is corroborated by polarization measurements of an individual ZPL excited with two distinct wavelengths that indicate a single ZPL may be excited by multiple mechanisms. These findings provide new insight on the nature of the optical cycle of novel defect-based single photon sources in h-BN. Comment: 21 pages, SI included. 5 figures |
Databáze: | OpenAIRE |
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