Compressive-Sensing-Enhanced First-Principles Calculation of Photoluminescence Spectra in Color Centers: A Comparison between Theory and Experiment for the G Center in Silicon
Jiongzhi Zheng, Lukasz Komza, Yihuang Xiong, Natalya Sheremetyeva, Changpeng Lin, Sinéad M. Griffin, Alp Sipahigil, Geoffroy Hautier
Photoluminescence (PL) spectra are a versatile tool for exploring the electronic and optical properties of quantum defect systems. In this work, we investigate the PL spectra of the G center in silicon by combining first-principles computations with a machine-learned compressive-sensing technique and experiment. We show that the compressive-sensing technique provides a speed up of approximately 20 times compared with the finite-displacement method with similar numerical accuracy. We compare theory and experiment and show good agreement for the historically proposed configuration B of the G center. In particular, we attribute the experimentally observed E-line of the G center to a local vibration mode mainly involving two substitutional C atoms and one interstitial Si atom. Our theoretical results also well reproduce and explain the experimental E-line energy shifts originating from the carbon isotopic effect. In addition, our results demonstrate that some highly anharmonic modes that are apparent in computed spectra could be absent experimentally because of their short lifetime. Our work not only provides a deeper understanding of the G-center defect but also paves the way to accelerate the calculation of PL spectra for color centers.
By coupling silicon nanowires (~150 nm diameter, 20 micron length) with an Ω-shaped plasmonic nanocavity we are able to generate broadband visible luminescence, which is induced by high-order hybrid nanocavity-surface plasmon modes. The nature of this super-bandgap emission is explored via photoluminescence spectroscopy studies performed with variable laser excitation energies (1.959 eV to 2.708 eV) and finite difference time domain simulations. Furthermore, temperature-dependent photoluminescence spectroscopy shows that the observed emission corresponds to radiative recombination of un-therma…
The room-temperature longitudinal piezoresistance of n-type and p-type crystalline silicon along selected crystal axes is investigated under uniaxial compressive stresses up to 3 GPa. While the conductance ($G$) of n-type silicon eventually saturates at $\approx 45%$ of its zero-stress value ($G_0$) in accordance with the charge transfer model, in p-type material $G/G_0$ increases above a predicted limit of $\approx 4.5$ without any significant saturation, even at 3 GPa. Calculation of $G/G_0$ using \textit{ab-initio} density functional theory reveals that neither $G$ nor the mobility, when pr…
Nanocomposite films of Zinc Oxide and Silicon were grown by thermal evaporation technique using varying ratios of ZnO:Si in the starting material. Analysis reveal the role of ZnO and amorphous silicon interface in contributing to relatively less common blue photoluminescence emissions (at $\sim$ 400 and 470nm). These blue peaks are observed along with the emissions resulting from band edge transition (370nm) and those related to defects (522nm) of ZnO. Careful analysis shows that along with the grain size of ZnO, a suitable compositional ratio (of ZnO to silicon) is critical for the coexistenc…
Silicon carbide with optically and magnetically active point defects offers unique opportunities for quantum technology applications. Since interaction with these defects commonly happens through optical excitation and de-excitation, a complete understanding of their light-matter interaction in general and optical signatures, in particular, is crucial. Here, we employ quantum mechanical density functional theory calculations to investigate the photoluminescence lineshapes of selected, experimentally observed color centers (including single vacancies, double vacancies, and vacancy impurity pair…
We propose a new variety of silicon quantum dots containing fullerene-derived hollows of nearly arbitrary symmetry. Conglomerate structures are designed by connecting the quantum dots through two kinds of junctions. The quantum confinement effect is investigated using semiempirical quantum-mechanical method. It is shown that within each family of quantum dots, the band gap and the stability are inversely proportional to the particle effective size. Quantum dots inherit a wide variety of structural and symmetry properties from their parent fullerenes. The conglomerates confine electrons like qu…
Photoluminescence is observed at room temperature from phonon-assisted band-to-band emission in Si (1.067 eV peak) using unpatterned bulk p-type silicon wafer samples that were spin-coated with Er-doped (6 at. %) silica-gel films (0.13 micron) and vacuum annealed; the strongest emission was obtained at ~700 degrees C. Comparative study of annealing behavior indicates two-orders of magnitude efficiency enhancement. Emission from Er+3 ions in the silica film is used to gauge relative emission strengths. Mechanisms for inducing emission from silicon utilizing stresses in sol-gel-films are discuss…
An electron spin resonance (ESR) and photoluminescence signal is observed in the as grown single crystal of stishovite indicating the presence of defects in the non-irradiated sample. Photoluminescence of the as received stishovite single crystals exhibits two main bands - a blue at 3 eV and an UV at 4.75 eV. Luminescence is excited in the range of optical transparency of stishovite (below 8.75 eV) and, therefore, is ascribed to defects. A wide range of decay kinetics under a pulsed excitation is observed. For the blue band besides the exponential decay with a time constant of about 18 μs an a…
Ge-on-Si structures in-situ doped with phosphorus or arsenic via metal organic chemical vapor deposition (MOCVD) were investigated. Surface roughness, strain, threading dislocation desnity, Si-Ge interdiffusion, dopant diffusion, and photoluminescence were characterized to study the impacts of defect annealing and Si substrate offcut effects on the Ge film quality and most importantly, the light emission properties. All samples have a smooth surface (roughness < 1.5 nm), and the Ge films have a small tensile strain of 0.2%. As-grown P and As-doped Ge films have threading dislocaiton densities …
The demand for single photon sources at $λ~=~1.54~μ$m, which follows from the consistent development of quantum networks based on commercial optical fibers, makes Er:O$_x$ centers in Si still a viable resource thanks to the optical transition of $Er^{3+}~:~^4I_{13/2}~\rightarrow~^4I_{15/2}$. Yet, to date, the implementation of such system remains hindered by its extremely low emission rate. In this Letter, we explore the room-temperature photoluminescence (PL) at the telecomm wavelength of very low implantation doses of $Er:O_x$ in $Si$. The emitted photons, excited by a $λ~=~792~nm$ laser in …
Multiscale Correlation of Morphological, Chemical, and Optical Properties in p-Type Porous Silicon
Escuela de Física and Centro de Investigación en Ciencia e Ingeniería de Materiales (CICIMA), Sede Rodrigo Facio, Universidad de Costa Rica（哥斯达黎加大学物理学院与材料科学与工程研究中心（CICIMA），罗德里戈法西奥校区）
We generate silicon vacancy related defects in high-quality epitaxial silicon carbide layers by means of electron irradiation. By controlling the irradiation fluence, the defect concentration is varied over several orders of magnitude. We establish the excitation profile for optical pumping of these defects and evaluate the optimum excitation wavelength of 770 nm. We also measure the photoluminescence dynamics at room temperature and find a monoexponential decay with a characteristic lifetime of 6.1 ns. The integrated photoluminescence intensity depends linear on the excitation power density u…
Photoluminescence of Femtosecond Laser-irradiated Silicon Carbide
RPTU University Kaiserslautern-Landau（凯泽斯劳滕-兰道莱布尼茨技术大学）；Universität des Saarlandes（萨尔兰州立大学）；Luxembourg Institute of Science and Technology (LIST)（卢森堡科学与技术研究所）；University of Luxembourg（卢森堡大学）；Institut für Oberflächen- und Schichttechnik GmbH（表面与薄膜技术研究所有限公司）
The molecular dynamics (MD) approach is an effective tool for investigating atomistic dynamical phenomena at the surface of materials under strong laser irradiation. Therefore, numerous laser ablation MD simulation studies have been conducted to date. However, in most MD studies, non-thermal and entropic effects via hot electrons on interatomic interactions that could cause significant differences in the simulation results are not considered. In this study, the MD simulation of the laser ablation of the Si surface was conducted using an interatomic potential whose parameters depended on the el…
The photoluminescence and spin properties of ensembles of color centers in silicon carbide are enhanced by fabricating optically isolated slab waveguide structures and carefully controlling annealing and cooling conditions. We find that the photoluminescence signal of an ensemble of implanted defects is enhanced in slab waveguides by an order of magnitude over identically implanted bulk defects. The slab waveguide-enhanced photoluminescence of several defect species is used to study recombination and diffusion in the presence of thermal annealing with both rapid quench cooling and a longer ret…
Mn-doped GaAs nanowires were grown in the self-catalytic growth mode on oxidized Si(100) surface by molecular beam epitaxy and characterized by scanning and transmission electron microscopy, Raman scattering, photoluminescence, cathodoluminescence, and electron transport measurements. The transmission electron microscopy studies evidenced the substantial accumulation of Mn inside the catalyzing Ga droplets at the top of the nanowires. Optical and transport measurements revealed that the limit of Mn content for self-catalysed growth of GaAs nanowires corresponds to the doping level, i.e., is mu…
Nanocomposite thin films of Zinc Oxide and Silicon were grown by co-evaporating powdered ZnO and Si. This resulted in nanocrystallites of ZnO being embedded in Silicon. The mismatch in crystal structures of constituent materials result in the ZnO nanocrystals to exist in a state of stress. This along with oxygen vacancies in the samples result in good Photoluminescence emission at 520nm. Also, Silicon background gave a photoluminescence emission at 620nm. The structure was found quite stable over time since the homgenously dispersed ZnO nanocrystals do not agglomerate. The nanocomposites promi…
The study of hexagonal silicon polytypes attracts special attention due to their unique physical properties compared to the traditional cubic phase of Si. Thus, for some hexagonal phases, a significant improvement in the emission properties has been demonstrated. In this work, the luminescent properties of SiO2/Si structures irradiated with Kr+ ions at different doses and annealed at 800 °C have been systematically investigated. For such structures, a photoluminescence line at ~ 1240 nm is observed and associated with the formation of hexagonal 9R-Si phase inclusions. It is found that the vari…
Silicon-vacancy (SiV) centers in diamond are promising systems for quantum information applications due to their bright single photon emission and optically accessible spin states. Furthermore, SiV centers in low-strain diamond are insensitive to pertubations of the dielectric environment, i.e. they show very weak spectral diffusion. This property renders ensembles of SiV centers interesting for sensing applications. We here report on photoluminescence excitation (PLE) spectroscopy on an SiV ensemble in a low strain, CVD-grown high quality diamond layer, where we measure the fine structure wit…
The study of defect centers in silicon has been recently reinvigorated by their potential applications in optical quantum information processing. A number of silicon defect centers emit single photons in the telecommunication $O$-band, making them promising building blocks for quantum networks between computing nodes. The two-carbon G-center, self-interstitial W-center, and spin-$1/2$ T-center are the most intensively studied silicon defect centers, yet despite this, there is no consensus on the precise configurations of defect atoms in these centers, and their electronic structures remain amb…
The negatively charged silicon vacancy ($\mathrm{V_{Si}^-}$) in silicon carbide is a well-studied point defect for quantum applications. At the same time, a closer inspection of ensemble photoluminescence and electron paramagnetic resonance measurements reveals an abundance of related but so far unidentified signals. In this study, we search for defects in 4H-SiC that explain the above magneto-optical signals in a defect database generated by Automatic Defect Analysis and Qualification (ADAQ) workflows. This search reveals only one class of atomic structures that exhibit silicon-vacancy-like p…
The silicon vacancy is a prominent intrinsic defect of cubic SiC (3C-SiC) to which much effort has been devoted so far, experimentally and theoretically. We calculate its properties using the GW approximation that does not suffer from the band gap problem. The obtained formation and transition energies deviate significantly from the usual density functional theory evaluations and now compare favorably with experiment. A new assignment for the main line of photoluminescence is then proposed. We further perform GW calculations for the saddle point of reaction paths. The resulting barrier energie…
Prior studies have shown that photoluminescence from Er3+ impurities in silicon is severely limited at room temperature by non-radiative relaxation and solid solubility; and room temperature emission from Er3+ in oxide-based hosts becomes diminished at high erbium concentrations. This work presents studies of thin films (0.2 micron thick) prepared by vacuum co-evaporation from elemental sources (Er, Si and Si/Ge) followed by vacuum annealing (600 degrees C); materials of this type, which are produced with high Er3+ concentrations, are shown to be capable of yielding strong room-temperature pho…
We report on the structure and electrical characteristics of silicon nanowire arrays prepared by metal assisted chemical etching (MACE) method, investigated by cross-sectional scanning electron microscopy (SEM) and high resolution X-ray diffraction (HR-XRD) methods. SEM micrographs show arrays of merged parallel nanowires, with lengths of 700 nm and 1000 nm, resulted after 1.5 min and 5 min etching time, respectively. X-ray reciprocal space maps (RSMs) around Si (004) reciprocal lattice point indicate the presence of 0D structural defects rather than of extended defects. The photoluminescence …
The features of some potential single-photon sources in two-dimensional silicon carbide monolayers is studied via ab-initio calculation and group theory analysis. A few point defects in three charge states (negative, positive and neutral) are considered. By applying performance criteria, Stone-Wales defects without and with combination of antisite defects are studied in details. The formation energy calculations reveal that neutral and positive charge states of these defects are stable. We compute the zero-phonon-line energy, the Huang-Rhys (HR) factor and the photoluminescence spectrum for th…
Silicon films doped with Er and O were prepared by techniques of physical vapor deposition on crystalline silicon, ion beam mixing and oxygen incorporation through Ar+ and O2+ implantation, and thermal annealing. Processing steps were tailored to be compatible with standard CMOS and to be of notably low cost to fabricate optically active media for silicon-based infrared emitters. The Si:Er:O films exhibit strong photoluminescence at room temperature that is analogous to Stark-split Er+3 ion 1.55-micron bands in fiber-optic materials. Concentration distributions were determined by Rutherford ba…
We report a giant thermal shift of $2.1 \,$MHz/K related to the excited-state zero-field splitting in the silicon vacancy centers in 4H silicon carbide. It is obtained from the indirect observation of the optically detected magnetic resonance in the excited state using the ground state as an ancilla. Alternatively, relative variations of the zero-field splitting for small temperature differences can be detected without application of radiofrequency fields, by simply monitoring the photoluminescence intensity in the vicinity of the level anticrossing. This effect results in an all-optical therm…
Bulk silicon carbide (SiC) is a very promising material system for bio-applications and quantum sensing. However, its optical activity lies beyond the near infrared spectral window for in-vivo imaging and fiber communications due to a large forbidden energy gap. Here, we report the fabrication of SiC nanocrystals and isolation of different nanocrystal fractions ranged from 600 nm down to 60 nm in size. The structural analysis reveals further fragmentation of the smallest nanocrystals into ca. 10-nm-size clusters of high crystalline quality, separated by amorphization areas. We use neutron irra…
The split silicon-vacancy defect (SiV) in diamond is an electrically and optically active color center. Recently, it has been shown that this color center is bright and can be detected at the single defect level. In addition, the SiV defect shows a non-zero electronic spin ground state that potentially makes this defect an alternative candidate for quantum optics and metrology applications beside the well-known nitrogen-vacancy color center in diamond. However, the electronic structure of the defect, the nature of optical excitations and other related properties are not well-understood. Here w…
Electrically driven emission from negatively charged silicon-vacancy, (SiV)- centres in single crystal diamond is demonstrated. The SiV centres were generated using ion implantation into an intrinsic (i) region of a p-i-n single crystal diamond diode. Both electroluminescence and the photoluminescence signals exhibit the typical emission that is attributed to the (SiV)- centres. Under forward and reversed biased PL measurements, no signal from the neutral (SiV)0 defect could be observed. The realization of electrically driven (SiV)- emission is promising for scalable nanophotonics devices empl…
We characterize a high-density sample of negatively charged silicon-vacancy (SiV$^-$) centers in diamond using collinear optical multidimensional coherent spectroscopy. By comparing the results of complementary signal detection schemes, we identify a hidden population of \ce{SiV^-} centers that is not typically observed in photoluminescence, and which exhibits significant spectral inhomogeneity and extended electronic $T_2$ times. The phenomenon is likely caused by strain, indicating a potential mechanism for controlling electric coherence in color-center-based quantum devices.
Confined microexplosions induced in silicon by powerful ultrashort laser pulses can lead to new Si phases. Some of these have not previously been observed via near-equilibrium compression of silicon. In this study, confocal Raman micro-spectroscopy and Raman imaging of arrays of microexplosions have been conducted to search for Raman signatures of these novel allotropes of silicon. A microexplosion is generated at the interface between a thick silicon dioxide confinement layer and underlying silicon. It is characterised by a void at the interface above a region of compressed silicon. Raman dat…
Silicon is host to two separate leading quantum technology platforms: integrated silicon photonics as well as long-lived spin qubits. There is an ongoing search for the ideal photon-spin interface able to hybridize these two approaches into a single silicon platform offering substantially expanded capabilities. A number of silicon defects are known to have spin-selective optical transitions, although very few of these are known to be in the highly desirable telecommunications bands, and those that do often do not couple strongly to light. Here we characterize the T center in silicon, a highly …
The electron spins of semiconductor defects can have complex interactions with their host, particularly in polar materials like SiC where electrical and mechanical variables are intertwined. By combining pulsed spin resonance with ab-initio simulations, we show that spin-spin interactions within SiC neutral divacancies give rise to spin states with an enhanced Stark effect, sub-10**-6 strain sensitivity, and highly spin-dependent photoluminescence with intensity contrasts of 15-36%. These results establish SiC color centers as compelling systems for sensing nanoscale fields.
The neutrally-charged silicon vacancy in diamond is a promising system for quantum technologies that combines high-efficiency, broadband optical spin polarization with long spin lifetimes (T2 ~ 1 ms at 4 K) and up to 90% of optical emission into its 946 nm zero-phonon line. However, the electronic structure of SiV0 is poorly understood, making further exploitation difficult. Performing photoluminescence spectroscopy of SiV0 under uniaxial stress, we find the previous excited electronic structure of a single 3A1u state is incorrect, and identify instead a coupled 3Eu - 3A2u system, the lower st…
Room-temperature 1535-nm-band photoluminescence in ~126 nm silica films (6 at. % doping), produced by spin-coating an Er2O3 and tetraethylorthosilicate sol-gel formulation on silicon substrates, was studied as a function of vacuum furnace annealing (500 to 1050 degrees C). Emission is strongly enhanced for annealing near 850 degrees C, which is shown by modeling the temperature dependence as arising from thermally-activated removal of hydroxyl ions. Suitability of such a process for silicon-based applications is discussed.
Silicon carbide has recently been developed as a platform for optically addressable spin defects. In particular, the neutral divacancy in the 4H polytype displays an optically addressable spin-1 ground state and near-infrared optical emission. Here, we present the Purcell enhancement of a single neutral divacancy coupled to a photonic crystal cavity. We utilize a combination of nanolithographic techniques and a dopant-selective photoelectrochemical etch to produce suspended cavities with quality factors exceeding 5,000. Subsequent coupling to a single divacancy leads to a Purcell factor of ~50…
Porous silicon (p-Si), prepared by two routes (metal induced etching (MIE) and laser induced etching (LIE)) have been studied by comparing the observed surface morphologies using SEM. A uniformly distributed smaller (submicron sized) pores are formed when MIE technique is used because the pore formation is driven by uniformly distributed metal (silver in present case) nanoparticles, deposited prior to the porosification step. Whereas in p-Si, prepared by LIE technique, wider pores with some variation in pore size as compared to MIE technique is observed because a laser having gaussian profile …
Photoluminescence (PL) spectra of single silicon vacancy (SiV) centers frequently feature very narrow room temperature PL lines in the near-infrared (NIR) spectral region, mostly between 820 nm and 840 nm, in addition to the well known zero-phonon-line (ZPL) at approx. 738 nm [E. Neu et al., Phys. Rev. B 84, 205211 (2011)]. We here exemplarily prove for a single SiV center that this NIR PL is due to an additional purely electronic transition (ZPL). For the NIR line at 822.7 nm, we find a room temperature linewidth of 1.4 nm (2.6 meV). The line saturates at similar excitation power as the ZPL. …
We develop ZnO/p-Si photodetectors by atomic layer deposition (ALD) of ZnO thin films on laser-microstructured silicon and we investigate their electrical and optical behavior, demonstrating high sensitivity and broadband operation. Microstructured p-type silicon was obtained by ns-laser irradiation in SF6 gas, which results in the formation of quasi-ordered and uniform microspikes on the silicon surface. The irradiated silicon contains sulfur impurities, which extend its absorbance to the near infrared. A thin film of ZnO was conformally deposited on the microstructured silicon substrates by …
Using molecular dynamics (MD) simulation, we investigate the mechanical response of silicon to high dose ion-irradiation. We employ a realistic and efficient model to directly simulate ion beam induced amorphization. Structural properties of the amorphized sample are compared with experimental data and results of other simulation studies. We find the behavior of the irradiated material is related to the rate at which it can relax. Depending upon the ability to deform, we observe either the generation of a high compressive stress and subsequent expansion of the material, or generation of tensil…
