Dielectric Loss due to Charged-Defect Acoustic Phonon Emission

The coherence times of state-of-the-art superconducting qubits are limited by bulk dielectric loss, yet the microscopic mechanism leading to this loss is unclear. Here we propose that the experimentally observed loss can be attributed to the presence of charged defects that enable the absorption of electromagnetic radiation by the emission of acoustic phonons. Our explicit derivation of the absorption coefficient for this mechanism allows us to derive a loss tangent of $7.2 \times 10^{-9}$ for Al$_2$O$_3$, in good agreement with recent high-precision measurements [A. P. Read et al., Phys. Rev. Appl. 19, 034064 (2023)]. We also find that for temperatures well below ~0.2 K, the loss should be independent of temperature, also in agreement with observations. Our investigations show that the loss per defect depends mainly on properties of the host material, and a high-throughput search suggests that diamond, cubic BN, AlN, and SiC are optimal in this respect

Dangling Bonds in Hexagonal Boron Nitride as Single-Photon Emitters.

Hexagonal boron nitride has been found to host color centers that exhibit single-photon emission, but the microscopic origin of these emitters is unknown. We propose boron dangling bonds as the likely source of the observed single-photon emission around 2 eV. An optical transition where an electron is excited from a doubly occupied boron dangling bond to a localized B p_{z} state gives rise to a zero-phonon line of 2.06 eV and emission with a Huang-Rhys factor of 2.3. This transition is linearly polarized with the absorptive and emissive dipole aligned. Because of the energetic position of the states within the band gap, indirect excitation through the conduction band will occur for sufficiently large excitation energies, leading to the misalignment of the absorptive and emissive dipoles seen in experiment. Our calculations predict a singlet ground state and the existence of a metastable triplet state, in agreement with experiment

Trap-Assisted Auger-Meitner Recombination from First Principles

Trap-assisted nonradiative recombination is known to limit the efficiency of optoelectronic devices, but the conventional multi-phonon emission (MPE) process fails to explain the observed loss in wide-band-gap materials. Here we highlight the role of trap-assisted Auger-Meitner (TAAM) recombination, and present a first-principles methodology to determine TAAM rates due to defects or impurities in semiconductors or insulators. We assess the impact on efficiency of light emitters in a recombination cycle that may include both TAAM and carrier capture via MPE. We apply the formalism to the technologically relevant case study of a calcium impurity in InGaN, where a Shockley-Read-Hall recombination cycle involving MPE alone cannot explain the experimentally observed nonradiative loss. We find that, for band gaps larger than 2.5 eV, the inclusion of TAAM results in recombination rates that are orders of magnitude larger than recombination rates based on MPE alone, demonstrating that TAAM can be a dominant nonradiative process in wide-band-gap materials. Our computational formalism is general and can be applied to the calculation of TAAM rates in any semiconducting or insulating material

Probing the Optical Dynamics of Quantum Emitters in Hexagonal Boron Nitride

Hexagonal boron nitride is a van der Waals material that hosts visible-wavelength quantum emitters at room temperature. However, experimental identification of the quantum emitters' electronic structure is lacking, and key details of their charge and spin properties remain unknown. Here, we probe the optical dynamics of quantum emitters in hexagonal boron nitride using photon emission correlation spectroscopy. Several quantum emitters exhibit ideal single-photon emission with noise-limited photon antibunching, $g^{(2)}(0)=0$. The photoluminescence emission lineshapes are consistent with individual vibronic transitions. However, polarization-resolved excitation and emission suggests the role of multiple optical transitions, and photon emission correlation spectroscopy reveals complicated optical dynamics associated with excitation and relaxation through multiple electronic excited states. We compare the experimental results to quantitative optical dynamics simulations, develop electronic structure models that are consistent with the observations, and discuss the results in the context of ab initio theoretical calculations.Comment: 31 pages, 16 figures, 6 table

Quantum Defects from First Principles

Point defects in semiconductors or insulators are a promising platform to realize quantum information science, composed of quantum computing, quantum communication, and quantum metrology. These so-called quantum defects are particularly appealing because they are fixed in a controlled solid-state environment, hold the promise of room temperature operation, and will benefit from mature semiconductor fabrication techniques for integration and scaling. First-principles calculations based on density functional theory have been indispensable for the study of point defects: such calculations provide crucial microscopic insight that may be inaccessible in experiments. In this dissertation, we develop and apply first-principles methodologies to treat quantum defects.Nonradiative transitions are integral to the control and operation of quantum defects. Indeed, nonradiative transitions dissipate energy through vibrations and thus can impact the quantum efficiency of a given quantum defect. We developed the Nonrad code, which implements a quantum-mechanical formalism to evaluate the nonradiative transition rate from first principles. We also put into effect several important modifications that are essential for attaining accurate rates.Identifying novel quantum defects is of vital importance for their widespread utilization in quantum information science. Boron nitride is an ultra-wide-band-gap material with excellent thermal and chemical stability, making it a promising host for quantum defects and for applications in electronic devices. Control over conductivity is essential to utilize boron nitride in the proposed applications. In cubic boron nitride, we assess potential dopants and their ability to produce n-type conductivity.In hexagonal boron nitride, bright single-photon emitters have been observed in the visible spectrum; however the microscopic origin of the emission has eluded researchers. Here we propose boron dangling bonds as the origin of the emission and provide a thorough characterization of their properties. We find that boron dangling bonds possess an optical transition with minimal coupling to phonons; we also calculate the magnetic-field dependence and show it to be in agreement with experiments. In a monolayer, we find that the boron dangling bond will behave similarly to when it is embedded in bulk material. Furthermore, we demonstrate the importance of out-of-plane distortions on the dangling bond, a result that has implications for other quantum defects in two-dimensional materials. Finally, in a fruitful collaboration with the experimental group of Prof. Lee Bassett at the University of Pennsylvania, we elucidated the optical dynamics of boron dangling bonds.In total, this work advances the study of quantum defects through the development and application of first-principles techniques

Dielectric loss due to charged-defect acoustic phonon emission

The coherence times of state-of-the-art superconducting qubits are limited by bulk dielectric loss, yet the microscopic mechanism leading to this loss is unclear. Here, we propose that the experimentally observed loss can be attributed to the presence of charged defects that enable the absorption of electromagnetic radiation by the emission of acoustic phonons. Our explicit derivation of the absorption coefficient for this mechanism allows us to derive a loss tangent of 7.2 × 10−9 for Al2O3, in good agreement with recent high-precision measurements [Read et al., Phys. Rev. Appl. 19, 034064 (2023)]. We also find that for temperatures well below ∼0.2 K, the loss should be independent of temperature, which is also in agreement with observations. Our investigations show that the loss per defect depends mainly on properties of the host material, and a high-throughput search suggests that diamond, cubic BN, AlN, and SiC are optimal in this respect

Dimensionality effects on trap-assisted recombination: the Sommerfeld parameter

In the context of condensed matter physics, the Sommerfeld parameter describes the enhancement or suppression of free-carrier charge density in the vicinity of a charged center. The Sommerfeld parameter is known for three-dimensional systems and is integral to the description of trap-assisted recombination in solids. Here we derive the Sommerfeld parameter in one and two dimensions and compare with the results in three dimensions. We provide an approximate analytical expression for the Sommerfeld parameter in two dimensions. Our results indicate that the effect of the Sommerfeld parameter is to suppress trap-assisted recombination in decreased dimensionality