Silicon-28-Tetrafluoride as an Educt of Isotope-Engineered Silicon Compounds and Bulk Materials for Quantum Systems
Abstract
:1. Introduction
- (i)
- Spin vacuum: The coherence of the electron spin states is disrupted by the interference of nuclear spins, for instance, from 29Si nuclei, which results in the loss of functionality of the qubits [3]. Silicon crystals made of nuclear-spin-free stable isotopes like 28Si and 30Si are ideal for hosting spin quantum bits due to their coherent properties, which are not disrupted by host nuclear spins. The property known as spin vacuum results in sharp ensemble donor resonances and extended spin relaxation times [4]. In pure 28Si material, the theoretical maximum for qubit decoherence times is 10 h [5]. In addition to quantum computing, the 28Si spin vacuum is also employed to stabilize optically active quantum dots in silicon [6].
- (ii)
- High thermal conductivity: The phonon scattering and, consequently, the thermal conductivity are markedly changed at low temperatures in the isotopically pure materials [4,7]. The formation of scattering modes is primarily caused by the presence of impurities, doping agents, defects, and the natural mass distribution of isotopes. It is possible to reduce the impact of the former factors by optimizing the crystal growth and deposition processes. The thermal conductivity of high-purity, monocrystalline, low-defect natSi with a natural isotope distribution is 45 Wcm−1K−1 at a temperature of 21 K. With the use of isotopically pure 28Si, the thermal conductivity at 21 K can be increased to 450 Wcm−1K−1 when the material is 99.99% pure. This value exceeds the previous maximum conductivity of 12C diamond at 104 K of 410 Wcm−1K−1. Consequently, the highest thermal conductivity ever measured for a dielectric was achieved [7].
- (iii)
- Sharp spectroscopic states: The analysis of photoluminescence spectra indicates that the homogeneous mass of the 28Si atoms in the crystal lattice results in a shift of the band gap by 58 meV [8]. Furthermore, high-energy measurements reveal a more concise fine structure of the non-phononic photoluminescence lines of the bound excitons. The optimized fine structure in the photoluminescence spectrum can be used for excitonic processes in isotopically pure materials with high resolution, for example, for quantum sensing.
2. Chemical Properties and Processing of 28SiF4
2.1. Synthesis and Selected Properties of SiF4 (and 28SiF4)
2.1.1. Synthesis Routes and Formation of SiF4
2.1.2. Solid State, Gas Phase, and Electronic Structure of SiF4
2.1.3. Physical and Chemical Properties
Property | Symbol | Unit | Value | Reference |
---|---|---|---|---|
Melting point | mp | °C | −95.0 (sublm.) | [62] |
Boiling point | bp | K | 177.1 | [63] |
Critical temperature | TC | K | 259 | [64] |
Critical pressure | pC | bar | 37.1457 | [64] |
Vapor pressure | P° | Pa | 3.36 × 10⁵ (at 190 K) | [65] |
Heat capacity | C | J/molK | 73.621 | [66] |
Ionization potential | IE | eV | 15.29 ± 0.08 | [67] |
Bond dissociation energy (homolysis) | D0 | kJ/mol | 565 | [68] |
Appearance energy (heterolysis, SiF3+) | AE | eV | 16.2 ± 0.1 | [69] |
Standard enthalpy of formation | ΔHf | kJ/mol | −1615 (at 298 K) | [66] |
Standard entropy | S | J/molK | 282.76 (at 298 K) | [66] |
Viscosity | v | m2/s | 0.404 × 106 (at 300 K; 975 kPa) | [70] |
Density | ρ | g/cm3 | 0.00469 (at 760 mmHg) | [71] |
2.1.4. Isotope-Dependent Physical/Chemical Properties
2.1.5. Further Selected Properties of SiF4
2.2. Important Applications of SiF4
3. Enrichment
- (i)
- The vapor pressure of the substance must exceed 5−10 mmHg (≙ 0.7–1.3 kPa) as the majority of enrichment techniques require gaseous sources;
- (ii)
- The substance must not react chemically with the materials of the enrichment chamber. Enrichment techniques exploit the slight differences in the physical properties of different isotopes. To exploit these properties, the working gas is introduced into enrichment chambers, which are usually made of stainless steel or special high-temperature alloys;
- (iii)
- Most enrichment techniques exploit the mass-dependent inertia of the isotopes. For sufficient enrichment, the molecular mass of the molecules must not be less than 40 u. Higher molecular masses are usually associated with higher enrichment rates and lower energy consumption;
- (iv)
- During the enrichment process, the working gas is usually heated either purposefully or by unwanted dissipative processes. The substance to be enriched must have a sufficiently high thermal stability;
- (v)
- There should be no chemical reaction between the molecules of the working gas. Anion exchange or atom exchange would result in an incomplete enrichment. Any interaction between the molecules of the substance should be minimized.
3.1. Gas Centrifuge
3.2. Laser Separation
3.3. Gas Diffusion
3.4. Other and Discontinued Technologies
4. Conversion to Silanes and Solid Silicon
4.1. Conversion to Bulk 28Si via 28SiO2
4.2. Conversion to 28SiH4
4.3. Conversion to Bulk 28Si via 28SiH4
4.4. Conversion to Thin 28Si Layers
5. Novel Physical Properties of 28Si Resulting from Isotope Enrichment and Its Applications
5.1. Mass Distribution|Avogadro Project
5.2. Thermal Conductivity|Cryogenics
5.3. Nuclear Spin|Quantum Technologies
5.4. Further Selected Properties and Potential Applications
Author Contributions
Funding
Data Availability Statement
Conflicts of Interest
References
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Nucleon Number Si | Nucleon Number F/H | Isotopic Ratio | Molar Mass | |
---|---|---|---|---|
28SiF4 | 28 | 19 | 92.23% | 103.94 u |
29SiF4 | 29 | 19 | 4.67% | 104.94 u |
30SiF4 | 30 | 19 | 3.10% | 105.93 u |
28Si1H4 | 28 | 1 | 92.219(4)% | 32.01 u |
28Si2H4 | 28 | 2 | 0.010(6)% | 36.03 u |
29Si1H4 | 29 | 1 | 4.669(5)% | 33.01 u |
29Si2H4 | 29 | 2 | 0.000(5)% | 37.03 u |
30Si1H4 | 30 | 1 | 3.099(6)% | 34.00 u |
30Si2H4 | 30 | 2 | 0.000(4)% | 38.14 u |
natSi | 28Si | Reference | |
---|---|---|---|
Mass distribution | 92.2%—28 u | 100%—28 u | [102] |
4.7%—29 u | |||
3.1%—30 u | |||
Thermal conductivity @ 21 K | 45 Wcm−1K−1 | 450 Wcm−1K−1 | [7] |
Band gap | 1.12 eV | 1.06 eV | [8] |
Nuclear spin | I = 1/2; Ī = √3/2 ħ | I = 0; Ī = 0 ħ |
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Ernst, O.C.; Uebel, D.; Brendler, R.; Kraushaar, K.; Steudel, M.; Acker, J.; Kroke, E. Silicon-28-Tetrafluoride as an Educt of Isotope-Engineered Silicon Compounds and Bulk Materials for Quantum Systems. Molecules 2024, 29, 4222. https://doi.org/10.3390/molecules29174222
Ernst OC, Uebel D, Brendler R, Kraushaar K, Steudel M, Acker J, Kroke E. Silicon-28-Tetrafluoride as an Educt of Isotope-Engineered Silicon Compounds and Bulk Materials for Quantum Systems. Molecules. 2024; 29(17):4222. https://doi.org/10.3390/molecules29174222
Chicago/Turabian StyleErnst, Owen C., David Uebel, Roman Brendler, Konstantin Kraushaar, Max Steudel, Jörg Acker, and Edwin Kroke. 2024. "Silicon-28-Tetrafluoride as an Educt of Isotope-Engineered Silicon Compounds and Bulk Materials for Quantum Systems" Molecules 29, no. 17: 4222. https://doi.org/10.3390/molecules29174222