skip to main content

Attention:

The NSF Public Access Repository (NSF-PAR) system and access will be unavailable from 5:00 PM ET until 11:00 PM ET on Friday, June 21 due to maintenance. We apologize for the inconvenience.


This content will become publicly available on October 18, 2024

Title: Optical Dipole Structure and Orientation of GaN Defect Single-Photon Emitters
GaN has recently been shown to host bright, photostable, defect single-photon emitters in the 600–700 nm wavelength range that are promising for quantum applications. The nature and origin of these defect emitters remain elusive. In this work, we study the optical dipole structures and orientations of these defect emitters using the defocused imaging technique. In this technique, the far-field radiation pattern of an emitter in the Fourier plane is imaged to obtain information about the structure of the optical dipole moment and its orientation in 3D. Our experimental results, backed by numerical simulations, show that these defect emitters in GaN exhibit a single dipole moment that is oriented almost perpendicular to the wurtzite crystal c-axis. Data collected from many different emitters show that the angular orientation of the dipole moment in the plane perpendicular to the c-axis exhibits a distribution that shows peaks centered at the angles corresponding to the nearest Ga–N bonds and also at the angles corresponding to the nearest Ga–Ga (or N–N) directions. Moreover, the in-plane angular distribution shows little difference among defect emitters with different emission wavelengths in the 600–700 nm range. Our work sheds light on the nature and origin of these GaN defect emitters.  more » « less
Award ID(s):
1839196
NSF-PAR ID:
10502819
Author(s) / Creator(s):
; ; ; ;
Publisher / Repository:
ACS
Date Published:
Journal Name:
ACS Photonics
Volume:
10
Issue:
10
ISSN:
2330-4022
Page Range / eLocation ID:
3723 to 3729
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. We report the experimental resonance enhanced multiphoton ionization spectrum of isoquinoline between 315 and 310 nm, along with correlated electronic structure calculations on the ground and excited states of this species. This spectral region spans the origin transitions to a π–π* excited state, which previous work has suggested to be vibronically coupled with a lower lying singlet n–π* state. Our computational results corroborate previous density functional theory calculations that predict the vertical excitation energy for the n–π* state to be higher than the π–π* state; however, we find an increase in the C–N–C angle brings the n–π* state below the energy of the π–π* state. The calculations find two out-of-plane vibrational modes of the n–π* state, which may be brought into near resonance with the π–π* state as the C–N–C bond angle increases. Therefore, the C–N–C bond angle may be important in activating vibronic coupling between the states. We fit the experimental rotational contour with a genetic algorithm to determine the excited state rotational constants and orientation of the transition dipole moment. The fits show a mostly in-plane polarized transition, and the projection of the transition dipole moment in the a-b plane is about 84° away from the a axis. These results are consistent with the prediction of our electronic structure calculations for the transition dipole moment of the π–π* excited state.

     
    more » « less
  2. Abstract

    Single-photon defect emitters (SPEs), especially those with magnetically and optically addressable spin states, in technologically mature wide bandgap semiconductors are attractive for realizing integrated platforms for quantum applications. Broadening of the zero phonon line (ZPL) caused by dephasing in solid state SPEs limits the indistinguishability of the emitted photons. Dephasing also limits the use of defect states in quantum information processing, sensing, and metrology. In most defect emitters, such as those in SiC and diamond, interaction with low-energy acoustic phonons determines the temperature dependence of the dephasing rate and the resulting broadening of the ZPL with the temperature obeys a power law. GaN hosts bright and stable single-photon emitters in the 600–700 nm wavelength range with strong ZPLs even at room temperature. In this work, we study the temperature dependence of the ZPL spectra of GaN SPEs integrated with solid immersion lenses with the goal of understanding the relevant dephasing mechanisms. At temperatures below ~ 50 K, the ZPL lineshape is found to be Gaussian and the ZPL linewidth is temperature independent and dominated by spectral diffusion. Above ~ 50 K, the linewidth increases monotonically with the temperature and the lineshape evolves into a Lorentzian. Quite remarkably, the temperature dependence of the linewidth does not follow a power law. We propose a model in which dephasing caused by absorption/emission of optical phonons in an elastic Raman process determines the temperature dependence of the lineshape and the linewidth. Our model explains the temperature dependence of the ZPL linewidth and lineshape in the entire 10–270 K temperature range explored in this work. The ~ 19 meV optical phonon energy extracted by fitting the model to the data matches remarkably well the ~ 18 meV zone center energy of the lowest optical phonon band ($$E_{2}(low)$$E2(low)) in GaN. Our work sheds light on the mechanisms responsible for linewidth broadening in GaN SPEs. Since a low energy optical phonon band ($$E_{2}(low)$$E2(low)) is a feature of most group III–V nitrides with a wurtzite crystal structure, including hBN and AlN, we expect our proposed mechanism to play an important role in defect emitters in these materials as well.

     
    more » « less
  3. Defect-based single photon emitters play an important role in quantum information technologies. Quantum emitters in technologically mature direct wide bandgap semiconductors, such as nitrides, are attractive for on-chip photonic integration. GaN has recently been reported to host bright and photostable defect single photon emitters in the 600–700 nm wavelength range. Spectral diffusion caused by local electric field fluctuation around the emitter limits the photon indistinguishability, which is a key requirement for quantum applications. In this work, we investigate the spectral diffusion properties of GaN defect emitters integrated with a solid immersion lens, employing both spectral domain and time domain techniques through spectroscopy and photon autocorrelation measurements at cryogenic temperature. Our results show that the GaN defect emitter at 10 K exhibits a Gaussian line shape with a linewidth of ∼1 meV while the spectral diffusion characteristic time falls within the range of a few hundred nanoseconds to a few microseconds. We study the dependency of the spectral diffusion rate and Gaussian linewidth on the excitation laser power. Our work provides insight into the ultrafast spectral diffusion in GaN defect-based single photon emitter systems and contributes toward harnessing the potential of these emitters for applications, especially for indistinguishable single photon generation.

     
    more » « less
  4. Previously, the infrared permittivity tensor of monoclinic β-Ga 2 O 3 crystals has been determined using ellipsometry reflection measurements from two differently oriented monoclinic β-Ga 2 O 3 crystals with surfaces parallel to (010) and (−201). The (010) surface places the crystallographic a-c plane in the table of the instrument. The permittivity tensor consists of four complex values, and in order to compute it, four or more combinations of measurements are required at selected table rotations and incidence angles. However, the (010) orientation also places the transverse optical (TO) modes with Au symmetry parallel to the z-axis of the instrument, and we find that these modes are not fully excited and, hence, not measurable due to underlying selection rules. This makes additional measurements on surfaces other than (010) necessary. The second orientation has been the (−201) crystal, which places the crystallographic b axis in the plane of the table to access the transverse Au phonons. In prior work, the overall tensor has been determined by combining measurements of the two crystal orientations [Schubert et al., Phys. Rev. B 93, 125209 (2016)]. The goal of the work here is to find single crystal orientations for which all TO modes can be determined from measurements. The use of a set of measurements employed for such a single crystal is inextricably linked to the choice of incidence angles and table rotations. Consequently, determining suitable angles for these is linked to the selection of a crystal orientation, which is, therefore, an integral part of the overall goal. The TO contribution to the permittivity strongly dominates at or near the TO mode wavenumber resonances and, therefore, are used in this work to identify suitable orientations for a single crystal. Any such crystal orientation will also provide measurements useful to compute permittivity across the entire measured wavenumber range. In principle, any crystal orientation that does not place the direction of any TO mode at or near the z-axis may be suitable due to the underlying physics and mathematics of the problem. We discuss which of these measurement parameters contain the most sensitivity for the (111) orientation. For accuracy, we seek the best or very good orientations. Our investigation follows a previously demonstrated approach where at a single wavelength, the full tensor of an orthorhombic absorbing crystal was obtained from a low-symmetry surface of stibnite [Schubert and Dollase, Opt. Lett. 27, 2073 (2002)]. We discuss which of these measurement parameters contain the most sensitivity for the (111) orientation. The methods presented here will also be useful for other monoclinic materials as well as other materials of different crystal structures, including orthorhombic and triclinic materials. 
    more » « less
  5. null (Ed.)
    Two new alkali vanadate carbonates with divalent transition metals have been synthesized as large single crystals via a high-temperature (600 °C) hydrothermal technique. Compound I , Rb 2 Mn 3 (VO 4 ) 2 CO 3 , crystallizes in the trigonal crystal system in the space group P 3̄1 c , and compound II , K 2 Co 3 (VO 4 ) 2 CO 3 , crystallizes in the hexagonal space group P 6 3 / m . Both structures contain honeycomb layers and triangular lattices made from edge-sharing MO 6 octahedra and MO 5 trigonal bipyramids, respectively. The honeycomb and triangular layers are connected along the c -axis through tetrahedral [VO 4 ] groups. The MO 5 units are connected with each other by carbonate groups in the ab -plane by forming a triangular magnetic lattice. The difference in space groups between I and II was also investigated with Density Functional Theory (DFT) calculations. Single crystal magnetic characterization of I indicates three magnetic transitions at 77 K, 2.3 K, and 1.5 K. The corresponding magnetic structures for each magnetic transition of I were determined using single crystal neutron diffraction. At 77 K the compound orders in the MnO 6 -honeycomb layer in a Néel-type antiferromagnetic orientation while the MnO 5 triangular lattice ordered below 2.3 K in a colinear ‘up–up–down’ fashion, followed by a planar ‘Y’ type magnetic structure. K 2 Co 3 (VO 4 ) 2 CO 3 ( II ) exhibits a canted antiferromagnetic ordering below T N = 8 K. The Curie–Weiss fit (200–350 K) gives a Curie–Weiss temperature of −42 K suggesting a dominant antiferromagnetic coupling in the Co 2+ magnetic sublattices. 
    more » « less