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Strongly correlated states of transition metal spin defects: the case of an iron impurity in aluminum nitride

T0 review · 3 major / 5 minor · reviewed 2026-08-10 · deepseek-v4-flash

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Pith's one-line read Quantum embedding methods DMET and QDET accurately describe the strongly correlated ground and excited states of an iron impurity in aluminum nitride, and spin-flip TDDFT reproduces its measured photoluminescence spectrum.

desk verdict A solid, honest benchmark showing QDET and DMET can treat a TM impurity in AlN; the validation rests heavily on SF-TDDFT for the excited-state geometry, which a referee should ask to be checked independently. read the letter →

arxiv 2501.16280 v1 pith:XBDXDISD submitted 2025-01-27 cond-mat.str-el

Leon Otis , Yu Jin , Victor Wen-zhe Yu , Siyuan Chen , Laura Gagliardi , Giulia Galli This is my paper · ORCID
classification cond-mat.str-el PACS 71.55.-i71.15.-m78.55.-m
keywords ironimpurityaluminumnitridespindefectsquantumembeddingdensitymatrixtheorydefectspin-fliptime-dependentfunctionalphotoluminescence
verification ladder T0 review T1 audit T2 compute T3 formal

The pith

A machine-rendered reading of the paper's core claim, the machinery that carries it, and where it could break.

The reading

Defect spin qubits in wide-gap materials live or die on their excited-state physics, and transition metal impurities are the hardest cases because their $d$-electron states are strongly correlated. This paper takes iron substituting aluminum in aluminum nitride as a benchmark and asks whether two quantum embedding methods, DMET and QDET, can describe both the ground state and the lowest excited state quantitatively. It claims they can: with carefully chosen active spaces and correct double-counting corrections, both methods give adiabatic excitation energies for the lowest $^4E$ state within roughly 0.1--0.2 eV of the measured 1.30 eV zero-phonon line. The paper also claims that spin-flip TDDFT, used for excited-state geometries, reproduces the measured photoluminescence spectrum in detail. A sympathetic reader would take the paper to be establishing that a practical, convergent protocol now exists for computing strongly correlated spin-defect excitations from first principles.

What carries the argument

The load-bearing object is an effective Hamiltonian for a small active space of defect orbitals, $H_{\text{eff}} = \sum_{ij} t^{\text{eff}}_{ij} a^\dagger_i a_j + \frac{1}{2} \sum_{ijkl} v^{\text{eff}}_{ijkl} a^\dagger_i a^\dagger_j a_l a_k$, diagonalized at high level while embedded in a lower-level description of the host. QDET (a Green's-function-based embedding method) builds this Hamiltonian from a $G_0W_0$ calculation and solves it with full configuration interaction, using an exact double-counting correction instead of an approximate one; DMET (a wave-function-based embedding method) builds a fragment-plus-bath space from a restricted open-shell Hartree-Fock wave function through a Schmidt decomposition and solves it with CASSCF or NEVPT2. The active-space protocol carries the argument: start from the five Fe $3d$ orbitals, then add occupied states nearest the valence band maximum for QDET, or Fe--N bonding and virtual $d$ orbitals for DMET, until excitation energies converge. Spin-flip TDDFT supplies the missing piece the embedding methods cannot provide, namely excited-state geometries, and those geometries yield the Franck-Condon shifts and Huang-Rhys spectral densities used to compare with the measured zero-phonon line and photoluminescence shape.

What would settle it

Find the 1.30 eV line in a sample with independently known FeAl concentration and charge state and show it belongs to another center, or compute the $^4E$ excited-state geometry with a multireference gradient method and obtain a Franck-Condon shift outside 0.08--0.11 eV; either result would move the adiabatic energies away from the measured zero-phonon line and break the claimed agreement.

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Extended reading notes

Core claim

The paper's central claim is that quantum embedding methods can handle the strongly correlated physics of a transition metal impurity in an insulator, a regime where simpler treatments fail. For iron substituting aluminum in wurtzite AlN, both DMET and QDET reproduce the high-spin $^6A_1$ ground state and place the lowest excited quartet $^4E$ at adiabatic excitation energies of about 1.0--1.5 eV, bracketing the measured zero-phonon line at 1.30 eV. The paper asserts that this agreement is not accidental: QDET needs only the five Fe $3d$ orbitals plus a few states near the valence band maximum, while DMET needs a larger active space including Fe--N bonding orbitals, and both are stable with respect to supercell size and functional choice. It further claims that spin-flip TDDFT correctly assigns the emitting state as $^4E$ and reproduces the experimental photoluminescence line shape, whereas spin-polarized DFT does not, because it cannot describe the multi-determinant nature and symmetry-breaking relaxation of the quartet.

Load-bearing premise

The accuracy claim assumes the measured 1.30 eV spectral line is the lowest excited quartet to ground sextet transition of the isolated neutral FeAl defect, and that the spin-flip TDDFT excited-state geometry used for the vibrational correction is correct.

Editorial extensions

If this is right

  • Transition metal impurities in insulators, previously flagged as a difficult case for embedding approaches such as cRPA, become tractable when the active space is grown systematically and double counting is handled exactly.
  • QDET needs a minimal or near-minimal active space for this defect, while DMET needs a larger space including Fe--N bonding orbitals; the paper's protocol tells practitioners how to converge both.
  • Spin-flip TDDFT can supply reliable excited-state geometries and photoluminescence line shapes for strongly correlated spin defects, while spin-polarized DFT cannot, even when its excitation energy looks acceptable.
  • Adiabatic excitation energies suitable for comparison with zero-phonon-line experiments can be assembled from embedding vertical energies plus TDDFT Franck-Condon shifts, with errors of order 0.1--0.2 eV.
  • The same division of labor, embedding for vertical energies and spin-flip TDDFT for relaxation, can be applied to other qubit-candidate defects in wide-gap hosts.

Reading between the lines

Editorial extensions of the paper, not claims the author makes directly.

  • The paper leaves implicit that its QDET recipe, starting from the five Fe $3d$ orbitals and adding states near the valence band maximum, likely transfers to other $3d$ impurities in nitride and oxide hosts, while the DMET space will depend on local bonding.
  • The 0.08--0.11 eV Franck-Condon correction is supplied entirely by spin-flip TDDFT; benchmarking it against a correlated excited-state geometry for a similar $^4E$ defect is the most direct test of the paper's error budget.
  • A screening workflow suggested but not developed here would pair QDET vertical energies with spin-flip TDDFT geometries and line shapes, reserving DMET for cases needing a wave-function embedding analysis.
  • Because only one measured zero-phonon line anchors the comparison, additional optical data, for example from isotopically purified or co-doped samples, would test the calculated quartet manifold more strictly than the present single line.
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Editorial analysis

A structured set of objections, weighed in public.

Desk editor's note, referee report, and a circularity audit.

Referee Report

3 major / 5 minor

Summary. The paper studies the neutral iron substitutional impurity (FeAl) in wurtzite AlN as a test case for strongly correlated transition-metal defects in insulators. Using two quantum embedding methods, QDET and DMET (with CASSCF and NEVPT2 solvers), and spin-flip TDDFT, the authors compute the 6A1 ground state and the lowest 4E excited state. They report vertical excitation energies with systematic supercell-size and active-space convergence tests, convert them to adiabatic excitation energies using Franck-Condon shifts from spin-flip TDDFT, and compare with the experimental zero-phonon line at 1.30 eV. They further compute vibrationally resolved photoluminescence spectra and show that spin-flip TDDFT with the HSE functional reproduces the measured line shape, while spin-polarized DFT does not. The central claim is that the embedding methods, when properly converged and with double-counting corrections, reliably describe this correlated defect, and that spin-flip TDDFT provides accurate excited-state geometries and spectra.

Significance. If the results hold, the paper provides a valuable benchmark for quantum embedding methods on a challenging system where cRPA-based approaches had previously struggled. The systematic active-space protocol for QDET and the identification of the need for larger active spaces in DMET are useful practical guidance for defect calculations. The paper's strengths include the absence of any parameter fitted to the defect's experimental excitation energy, explicit convergence checks over supercell size and active-space size, and direct comparison with an external experimental zero-phonon line and photoluminescence spectrum. The open-source implementations (pDMET and WEST) are also a plus for reproducibility. The experimental agreement within roughly 0.1-0.2 eV for NEVPT2-DMET, QDET, and hybrid TDDFT, together with the successful PL line shape, would support the usefulness of these methods for transition-metal defects in wide-gap insulators.

major comments (3)
  1. [Abstract; Table 1] The abstract claims that 'both DMET and QDET accurately describe the ground state and low-lying excited states,' but Table 1 shows CAS-DMET(15e,15o) giving an adiabatic excitation energy of 1.94 eV, which is 0.64 eV above the experimental ZPL and outside the stated 0.1-0.2 eV accuracy. Only NEVPT2-DMET is accurate. The claim should be qualified to 'DMET with a post-CASSCF correction' or 'NEVPT2-DMET,' and the abstract should not imply that the bare CASSCF-based DMET used here is accurate for this defect.
  2. [Table 1 and text near 'From the results reported in Table 1'] The construction of the adiabatic excitation energies is not fully transparent. The text says that Franck-Condon shifts from TDDFT@PBE (0.11 eV) are used, but it also reports HSE and DDH shifts of 0.08 eV, and Table 1 lists EFC,ES only for the PBE-TDDFT row. To make the comparison reproducible, the table should report the vertical excitation energy and the functional-specific Franck-Condon shift used for every method, and the text should explicitly state whether a common shift was applied to the QDET/NEVPT2-DMET entries or whether functional-specific shifts were used.
  3. [Figure 5(b); section 'To assess the accuracy...'] The accuracy of every AEE in Table 1 depends on the spin-flip TDDFT excited-state geometry, since the Franck-Condon shift is obtained from that geometry. The paper should explicitly state that the agreement of the computed PL line shape with experiment in Fig. 5(b), which is governed by Huang-Rhys factors and phonon energies, provides an independent experimental check of that geometry. It should also discuss the sensitivity of the result to the functional choice: PBE gives a shift of 0.11 eV while HSE and DDH give 0.08 eV, a spread of 0.03 eV that is comparable to the claimed accuracy of the embedding methods.
minor comments (5)
  1. [Introduction / assignment of experimental ZPL] The comparison in Table 1 relies on assigning the 1.30 eV zero-phonon line to the 4E -> 6A1 transition of the isolated neutral FeAl defect. The paper cites Ref. 25 for the measurement but does not discuss the evidence for this assignment; a brief justification or a citation to a review that establishes the assignment would strengthen the validation.
  2. [Figure 5(b) caption] The caption states that the computed spectra are horizontally shifted to align the ZPL with experiment. Please state explicitly that this comparison validates the line shape and Huang-Rhys factors, not the absolute transition energy.
  3. [Abstract] The statement 'TDDFT yields photoluminescence spectra in agreement with experiments' should be qualified to 'spin-flip TDDFT with the HSE or DDH functional,' since the Supporting Information shows that PBE gives a significantly larger Huang-Rhys factor (S_total = 5.73 vs 3.24 for HSE) and a correspondingly poorer line shape.
  4. [Table 1] The columns EFC,GS and EFC,ES are populated only for the PBE-TDDFT row. For readability, the caption should explain that these columns apply to the row shown, or the values should be listed for each functional family.
  5. [Section 'We now turn to exploring larger active spaces'] The description of the QDET active spaces as '(7e,6o), (19e,12o), and (51e,28o)' is clear, but the reader would benefit from a sentence explaining why adding occupied valence bands increases the electron count by the stated amounts; the current text implies this without giving the counting rule.

Circularity Check

0 steps flagged · score 2.0 of 10

No construction-level circularity: excitation energies are un-fitted calculations benchmarked against an external 1.30 eV ZPL; the only flagged item is the in-preparation Ref 35 self-citation used for QDET's double-counting and active-space protocol.

full rationale

The paper's central numerical claims do not reduce to their inputs. Table 1 is built as AEE = VEE(method) - E_FC,ES (SF-TDDFT), with VEEs from QDET, DMET, or TDDFT and the Franck-Condon shift from an independent geometry optimization; neither quantity is fitted to the experimental 1.30 eV zero-phonon line, and the resulting AEEs (1.02-1.50 eV for all methods except CAS-DMET) scatter around rather than equal the experimental value. The QDET and DMET vertical excitation energies are converged in supercell size and active space (Figures 2-4) before comparison. The shared use of SF-TDDFT for both the Franck-Condon shifts and the photoluminescence line shape means the geometry validation and the ZPL comparison are not fully independent, but this is a robustness/assumption concern, not an equality-by-construction or fitted-parameter circularity. The one self-citation worth noting is Ref 35, an in-preparation manuscript by the same group (Chen, Yu, Jin, Govoni, Galli), cited as the source of QDET's 'exact double counting correction' and of the active-space protocol; if that correction is not publicly available, reproducibility is limited, but the accuracy claim is externally benchmarked and does not collapse into that citation. Hence no significant circularity; score 2 reflects the minor in-preparation self-citation rather than a forced prediction.

Assumptions & free parameters 0 free parameters · 5 assumptions · 0 invented entities

The central claims rest on no fitted parameters, but on several domain assumptions about the experimental assignment, the charge state, and the accuracy of the spin-flip TDDFT geometries used to correct the embedding energies. The main methodological unknowns are the unpublished QDET double counting formalism and the active-space sensitivity of DMET.

assumptions (5)
  • domain assumption The neutral charge state of FeAl is the charge state relevant to the studied photoluminescence.
    The paper cites Ref 3 (Wickramaratne et al.) for the neutral state being lowest in energy; if the 1.30 eV emission came from a different charge state, the comparison would be invalid.
  • domain assumption The experimental ZPL at 1.30 eV (Ref 25) corresponds to the 4E to 6A1 transition of the isolated neutral FeAl defect.
    All accuracy assessments for the embedding methods rest on this assignment; Ref 25 is a 1994 measurement with limited spectroscopic characterization.
  • domain assumption Vibrational zero-point energy differences between the 6A1 and 4E states cancel when approximating the ZPL as the adiabatic excitation energy.
    Stated in the main text before Table 1; if the zero-point difference is tens of meV, the reported errors shift by that amount.
  • domain assumption Spin-flip TDDFT accurately describes the 4E excited-state geometry and the Franck-Condon shifts used to convert vertical excitation energies from DMET and QDET into adiabatic energies.
    The Franck-Condon shifts (0.08 to 0.11 eV) come from spin-flip TDDFT; a wrong excited-state relaxation would shift all AEE values in Table 1.
  • standard math The FCI solver in QDET and the CASSCF and NEVPT2 solvers in DMET are exact for the chosen active spaces, and the G0W0 and ROHF low-level descriptions are adequate.
    Standard assumptions of quantum embedding; the paper's active-space convergence studies mitigate this assumption for the 4E state.

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Pith. "Pith review of Strongly correlated states of transition metal spin defects: the case of an iron impurity in aluminum nitride." pith.science (2026). https://pith.science/paper/XBDXDISD

@misc{pith2026250116280,
  author       = {Pith},
  title        = {Pith review of: Strongly correlated states of transition metal spin defects: the case of an iron impurity in aluminum nitride},
  year         = {2026},
  howpublished = {\url{https://pith.science/paper/XBDXDISD}},
  note         = {Machine review of arXiv:2501.16280}
}
read the original abstract

We investigate the electronic properties of an exemplar transition metal impurity in an insulator, with the goal of accurately describing strongly correlated, defect states. We consider iron in aluminum nitride, a material of interest for hybrid quantum technologies, and we carry out calculations with quantum embedding methods -- density matrix embedding theory (DMET) and quantum defect embedding theory (QDET) and with spin-flip time-dependent density functional theory (TDDFT). We show that both DMET and QDET accurately describe the ground state and low-lying excited states of the defect, and that TDDFT yields photoluminescence spectra in agreement with experiments. In addition, we provide a detailed discussion of the convergence of our results as a function of the active space used in the embedding methods, thus defining a protocol to obtain converged data, directly comparable with experiments.

Figures

Figures reproduced from arXiv: 2501.16280 by the authors.

Figure 1
Figure 1. (a) Depiction of the Fe (yellow sphere) impurity in AlN. Al and N atoms are rep [PITH_FULL_IMAGE:figures/full_fig_p004_1.png] view at source ↗
Figure 2
Figure 2. Vertical excitation energies of the lowest [PITH_FULL_IMAGE:figures/full_fig_p009_2.png] view at source ↗
Figure 3
Figure 3. Vertical excitation energies of the lowest [PITH_FULL_IMAGE:figures/full_fig_p010_3.png] view at source ↗
Figures from the paper (3 more)
Figure 4
Figure 4. Figure 4: Vertical excitation energies of the lowest [PITH_FULL_IMAGE:figures/full_fig_p011_4.png]
Figure 5
Figure 5. Figure 5: (a) Schematic representation of the relationship between the vertical excitation en [PITH_FULL_IMAGE:figures/full_fig_p012_5.png]
Figure 6
Figure 6. Figure 6: Partial Huang-Rhys factors (Sk, red lines) and the spectral density (S(¯hω), blue line), for the 4E → 6A1 transition calculated using spin-flip TDDFT with the HSE functional. The spectral density is defined as S(¯hω) = P k Skδ(¯hω − hω¯ k). Vibrational modes that contr…

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Works this paper leans on

80 extracted references · 71 canonical work pages · cited by 1 Pith paper

  1. [1]

    B.; Janotti, A.; Van de Walle, C

    Varley, J. B.; Janotti, A.; Van de Walle, C. G. Defects in AlN as candidates for solid-state qubits. Phys. Rev. B 2016, 93, 161201

    work page 2016

  2. [2]

    J.; Anderson, C

    Wolfowicz, G.; Heremans, F. J.; Anderson, C. P.; Kanai, S.; Seo, H.; Gali, A.; Galli, G.; Awschalom, D. D. Quantum guidelines for solid-state spin defects. Nat. Rev. Mater. 2021, 6, 906--925

    work page 2021

  3. [3]

    E.; Alkauskas, A.; Van de Walle, C

    Wickramaratne, D.; Shen, J.-X.; Dreyer, C. E.; Alkauskas, A.; Van de Walle, C. G. Electrical and optical properties of iron in GaN, AlN, and InN. Phys. Rev. B 2019, 99, 205202

    work page 2019

  4. [4]

    Freysoldt, C.; Grabowski, B.; Hickel, T.; Neugebauer, J.; Kresse, G.; Janotti, A.; Van de Walle, C. G. First-principles calculations for point defects in solids. Rev. Mod. Phys. 2014, 86, 253--305

    work page 2014

  5. [5]

    E.; Alkauskas, A.; Lyons, J

    Dreyer, C. E.; Alkauskas, A.; Lyons, J. L.; Janotti, A.; Van de Walle, C. G. First-principles calculations of point defects for quantum technologies. Ann. Rev. Mater. Res. 2018, 48, 1--26

    work page 2018

  6. [6]

    Quantum simulations of materials on near-term quantum computers

    Ma, H.; Govoni, M.; Galli, G. Quantum simulations of materials on near-term quantum computers. npj Comput. Mater. 2020, 6, 85

    work page 2020

  7. [7]

    Green's function formulation of quantum defect embedding theory

    Sheng, N.; Vorwerk, C.; Govoni, M.; Galli, G. Green's function formulation of quantum defect embedding theory. J. Chem. Theory Comput. 2022, 18, 3512--3522

    work page 2022

  8. [8]

    Q.; Pandharkar, R.; Hermes, M

    Mitra, A.; Pham, H. Q.; Pandharkar, R.; Hermes, M. R.; Gagliardi, L. Excited states of crystalline point defects with multireference density matrix embedding theory. J. Phys. Chem. Lett. 2021, 12, 11688--11694

    work page 2021

Show all 80 references
  1. [9]

    R.; Gagliardi, L

    Haldar, S.; Mitra, A.; Hermes, M. R.; Gagliardi, L. Local excitations of a charged nitrogen vacancy in diamond with multireference density matrix embedding theory. J. Phys. Chem. Lett. 2023, 14, 4273--4280

    2023

  2. [10]

    R.; Gagliardi, L

    Mitra, A.; Hermes, M. R.; Gagliardi, L. Density matrix embedding using multiconfiguration pair-density functional theory. J. Chem. Theory Comput. 2023, 19, 3498--3508

    2023

  3. [11]

    R.; Galli, G.; Gagliardi, L

    Verma, S.; Mitra, A.; Jin, Y.; Haldar, S.; Vorwerk, C.; Hermes, M. R.; Galli, G.; Gagliardi, L. Optical properties of neutral F centers in bulk MgO with density matrix embedding . J. Phys. Chem. Lett. 2023, 7703--7710

    2023

  4. [12]

    W.-z.; Govoni, M.; Xu, A

    Jin, Y.; Yu, V. W.-z.; Govoni, M.; Xu, A. C.; Galli, G. Excited state properties of point defects in semiconductors and insulators investigated with time-dependent density functional theory. J. Chem. Theory Comput. 2023, 19, 8689--8705

    2023

  5. [13]

    Quantum embedding theories to simulate condensed systems on quantum computers

    Vorwerk, C.; Sheng, N.; Govoni, M.; Huang, B.; Galli, G. Quantum embedding theories to simulate condensed systems on quantum computers. Nat. Comput. Sci. 2022, 2, 424--432

    2022

  6. [14]

    Sun, Q.; Chan, G. K.-L. Quantum embedding theories . Acc. Chem. Res. 2016, 49, 2705--2712

    2016

  7. [15]

    Quantum embedding theory for strongly correlated states in materials

    Ma, H.; Sheng, N.; Govoni, M.; Galli, G. Quantum embedding theory for strongly correlated states in materials. J. Chem. Theory Comput. 2021, 17, 2116--2125

    2021

  8. [16]

    I.; Hampel, A.; Cano, J.; R\"osner, M.; Dreyer, C

    Muechler, L.; Badrtdinov, D. I.; Hampel, A.; Cano, J.; R\"osner, M.; Dreyer, C. E. Quantum embedding methods for correlated excited states of point defects: Case studies and challenges. Phys. Rev. B 2022, 105, 235104

    2022

  9. [17]

    Disentangling photoexcitation and photoluminescence processes in defective MgO

    Vorwerk, C.; Galli, G. Disentangling photoexcitation and photoluminescence processes in defective MgO. Phys. Rev. Mater. 2023, 7, 033801

    2023

  10. [18]

    R.; Koehl, W

    Weber, J. R.; Koehl, W. F.; Varley, J. B.; Janotti, A.; Buckley, B. B.; de Walle, C. G. V.; Awschalom, D. D. Quantum computing with defects. Proc. Natl. Acad. Sci. USA 2010, 107, 8513--8518

    2010

  11. [19]

    B.; Nakarmi, M

    Li, J.; Nam, K. B.; Nakarmi, M. L.; Lin, J. Y.; Jiang, H. X.; Carrier, P.; Wei, S.-H. Band structure and fundamental optical transitions in wurtzite AlN. Appl. Phys. Lett. 2003, 83, 5163--5165

    2003

  12. [20]

    AlN piezoelectric thin films for energy harvesting and acoustic devices

    Fei, C.; Liu, X.; Zhu, B.; Li, D.; Yang, X.; Yang, Y.; Zhou, Q. AlN piezoelectric thin films for energy harvesting and acoustic devices. Nano Energy 2018, 51, 146--161

    2018

  13. [21]

    L.; Klimov, P

    Falk, A. L.; Klimov, P. V.; Buckley, B. B.; Iv\'ady, V.; Abrikosov, I. A.; Calusine, G.; Koehl, W. F.; Gali, A.; Awschalom, D. D. Electrically and mechanically tunable electron spins in silicon carbide color centers. Phys. Rev. Lett. 2014, 112, 187601

    2014

  14. [22]

    Designing defect-based qubit candidates in wide-gap binary semiconductors for solid-state quantum technologies

    Seo, H.; Ma, H.; Govoni, M.; Galli, G. Designing defect-based qubit candidates in wide-gap binary semiconductors for solid-state quantum technologies. Phys. Rev. Mater. 2017, 1, 075002

    2017

  15. [23]

    Sohn, Y.-I. et al. Controlling the coherence of a diamond spin qubit through its strain environment. Nat. Commun. 2018, 9, 2012

    2018

  16. [24]

    Malguth, E.; Hoffmann, A.; Phillips, M. R. Fe in III–V and II–VI semiconductors. Phys. Status Solidi b 2008, 245, 455--480

    2008

  17. [25]

    Determination of the GaN/AlN band offset via the (‐/0) acceptor level of iron

    Baur, J.; Maier, K.; Kunzer, M.; Kaufmann, U.; Schneider, J. Determination of the GaN/AlN band offset via the (‐/0) acceptor level of iron. Appl. Phys. Lett. 1994, 65, 2211--2213

    1994

  18. [26]

    G.; Neugebauer, J

    Van de Walle, C. G.; Neugebauer, J. First-principles calculations for defects and impurities: Applications to III-nitrides. J. Appl. Phys. 2004, 95, 3851--3879

    2004

  19. [27]

    G.; Chen, Y.; Zhu, Z

    Tu, Y.; Tang, Z.; Zhao, X. G.; Chen, Y.; Zhu, Z. Q.; Chu, J. H.; Fang, J. C. A paramagnetic neutral V_ Al O_N center in wurtzite AlN for spin qubit application. Appl. Phys. Lett. 2013, 103, 072103

    2013

  20. [28]

    Design of defect spins in piezoelectric aluminum nitride for solid-state hybrid quantum technologies

    Seo, H.; Govoni, M.; Galli, G. Design of defect spins in piezoelectric aluminum nitride for solid-state hybrid quantum technologies. Sci. Rep. 2016, 6, 20803

    2016

  21. [29]

    Electronic structure of transition metal ions in GaN and AlN: Comparing GGA+U with experiment

    Zakrzewski, T.; Boguslawski, P. Electronic structure of transition metal ions in GaN and AlN: Comparing GGA+U with experiment. J. Alloy. Compd. 2016, 664, 565--579

    2016

  22. [30]

    Aryasetiawan, F.; Imada, M.; Georges, A.; Kotliar, G.; Biermann, S.; Lichtenstein, A. I. Frequency-dependent local interactions and low-energy effective models from electronic structure calculations. Phys. Rev. B 2004, 70, 195104

    2004

  23. [31]

    Ab initio description of highly correlated states in defects for realizing quantum bits

    Bockstedte, M.; Sch \"u tz, F.; Garratt, T.; Iv \'a dy, V.; Gali, A. Ab initio description of highly correlated states in defects for realizing quantum bits. npj Quantum Mater. 2018, 3, 31

    2018

  24. [32]

    Knizia, G.; Chan, G. K.-L. Density matrix embedding: A simple alternative to dynamical mean-field theory. Phys. Rev. Lett. 2012, 109, 186404

    2012

  25. [33]

    Knizia, G.; Chan, G. K.-L. Density matrix embedding: A strong-coupling quantum embedding theory. J. Chem. Theory Comput. 2013, 9, 1428--1432

    2013

  26. [34]

    A.; Sun, Q.; Chan, G

    Wouters, S.; Jiménez-Hoyos, C. A.; Sun, Q.; Chan, G. K.-L. A practical guide to density matrix embedding theory in quantum chemistry. J. Chem. Theory Comput. 2016, 12, 2706--2719

    2016

  27. [35]

    W.-z.; Jin, Y.; Govoni, M.; Galli, G

    Chen, S.; Yu, V. W.-z.; Jin, Y.; Govoni, M.; Galli, G. New double counting formalism and hybridization in quantum defect embedding theory. In preparation, 2025

    2025

  28. [36]

    First-principles studies of strongly correlated states in defect spin qubits in diamond

    Ma, H.; Sheng, N.; Govoni, M.; Galli, G. First-principles studies of strongly correlated states in defect spin qubits in diamond. Phys. Chem. Chem. Phys. 2020, 22, 25522--25527

    2020

  29. [37]

    Maximally localized generalized Wannier functions for composite energy bands

    Marzari, N.; Vanderbilt, D. Maximally localized generalized Wannier functions for composite energy bands. Phys. Rev. B 1997, 56, 12847--12865

    1997

  30. [38]

    A.; Yates, J

    Marzari, N.; Mostofi, A. A.; Yates, J. R.; Souza, I.; Vanderbilt, D. Maximally localized Wannier functions: Theory and applications. Rev. Mod. Phys. 2012, 84, 1419--1475

    2012

  31. [39]

    O.; Taylor, P

    Roos, B. O.; Taylor, P. R.; Sigbahn, P. E. A complete active space SCF method (CASSCF) using a density matrix formulated super-CI approach. Chem. Phys. 1980, 48, 157--173

    1980

  32. [40]

    A comparison of the super-CI and the Newton-Raphson scheme in the complete active space SCF method

    Siegbahn, P.; Heiberg, A.; Roos, B.; Levy, B. A comparison of the super-CI and the Newton-Raphson scheme in the complete active space SCF method. Phys. Scripta 1980, 21, 323

    1980

  33. [41]

    Siegbahn, P. E. M.; Alml\" o f, J.; Heiberg, A.; Roos, B. O. The complete active space SCF (CASSCF) method in a Newton–Raphson formulation with application to the HNO molecule. J. Chem. Phys. 1981, 74, 2384--2396

    1981

  34. [42]

    Introduction of n-electron valence states for multireference perturbation theory

    Angeli, C.; Cimiraglia, R.; Evangelisti, S.; Leininger, T.; Malrieu, J.-P. Introduction of n-electron valence states for multireference perturbation theory. J. Chem. Phys. 2001, 114, 10252--10264

    2001

  35. [43]

    N-electron valence state perturbation theory: A fast implementation of the strongly contracted variant

    Angeli, C.; Cimiraglia, R.; Malrieu, J.-P. N-electron valence state perturbation theory: A fast implementation of the strongly contracted variant. Chem. Phys. Lett. 2001, 350, 297--305

    2001

  36. [44]

    n-electron valence state perturbation theory: A spinless formulation and an efficient implementation of the strongly contracted and of the partially contracted variants

    Angeli, C.; Cimiraglia, R.; Malrieu, J.-P. n-electron valence state perturbation theory: A spinless formulation and an efficient implementation of the strongly contracted and of the partially contracted variants. J. Chem. Phys. 2002, 117, 9138--9153

    2002

  37. [45]

    A quasidegenerate formulation of the second order n-electron valence state perturbation theory approach

    Angeli, C.; Borini, S.; Cestari, M.; Cimiraglia, R. A quasidegenerate formulation of the second order n-electron valence state perturbation theory approach. J. Chem. Phys. 2004, 121, 4043--4049

    2004

  38. [46]

    Q.; Hermes, M

    Pham, H. Q.; Hermes, M. R.; Gagliardi, L. Periodic electronic structure calculations with the density matrix embedding theory. J. Chem. Theory Comput. 2020, 16, 130--140

    2020

  39. [47]

    Excited state nuclear forces from the Tamm–Dancoff approximation to time-dependent density functional theory within the plane wave basis set framework

    Hutter, J. Excited state nuclear forces from the Tamm–Dancoff approximation to time-dependent density functional theory within the plane wave basis set framework. J. Chem. Phys. 2003, 118, 3928--3934

    2003

  40. [48]

    Shao, Y.; Head-Gordon, M.; Krylov, A. I. The spin–flip approach within time-dependent density functional theory: Theory and applications to diradicals. J. Chem. Phys. 2003, 118, 4807--4818

    2003

  41. [49]

    Time-dependent density functional theory based on a noncollinear formulation of the exchange-correlation potential

    Wang, F.; Ziegler, T. Time-dependent density functional theory based on a noncollinear formulation of the exchange-correlation potential. J. Chem. Phys. 2004, 121, 12191--12196

    2004

  42. [50]

    Theoretical and numerical assessments of spin-flip time-dependent density functional theory

    Li, Z.; Liu, W. Theoretical and numerical assessments of spin-flip time-dependent density functional theory. J. Chem. Phys. 2012, 136, 024107

    2012

  43. [51]

    A.; Shao, Y.; Krylov, A

    Bernard, Y. A.; Shao, Y.; Krylov, A. I. General formulation of spin-flip time-dependent density functional theory using non-collinear kernels: Theory, implementation, and benchmarks. J. Chem. Phys. 2012, 136, 204103

    2012

  44. [52]

    Casanova, D.; Krylov, A. I. Spin-flip methods in quantum chemistry. Phys. Chem. Chem. Phys. 2020, 22, 4326--4342

    2020

  45. [53]

    Large scale GW calculations

    Govoni, M.; Galli, G. Large scale GW calculations. J. Chem. Theory Comput. 2015, 11, 2680--2696

    2015

  46. [54]

    W.-z.; Govoni, M

    Yu, V. W.-z.; Govoni, M. GPU acceleration of large-scale full-frequency GW calculations. J. Chem. Theory Comput. 2022, 18, 4690--4707

    2022

  47. [55]

    Vibrationally resolved optical excitations of the nitrogen-vacancy center in diamond

    Jin, Y.; Govoni, M.; Galli, G. Vibrationally resolved optical excitations of the nitrogen-vacancy center in diamond. npj Comput. Mater. 2022, 8, 238

    2022

  48. [56]

    Crystal structure refinement of AlN and GaN

    Schulz, H.; Thiemann, K. Crystal structure refinement of AlN and GaN. Solid State Commun. 1977, 23, 815--819

    1977

  49. [57]

    Giannozzi, P. et al. QUANTUM ESPRESSO: A modular and open-source software project for quantum simulations of materials. J. Phys. Condens. Mat. 2009, 21, 395502

    2009

  50. [58]

    Giannozzi, P. et al. Advanced capabilities for materials modelling with Quantum ESPRESSO. J. Phys. Condens. Mat. 2017, 29, 465901

    2017

  51. [59]

    F.; Ferretti, A.; Marzari, N.; Timrov, I.; Urru, A.; Baroni, S

    Giannozzi, P.; Baseggio, O.; Bonf\` a , P.; Brunato, D.; Car, R.; Carnimeo, I.; Cavazzoni, C.; de Gironcoli, S.; Delugas, P.; Ruffino, F. F.; Ferretti, A.; Marzari, N.; Timrov, I.; Urru, A.; Baroni, S. Quantum ESPRESSO toward the exascale. J. Chem. Phys. 2020, 152, 154105

    2020

  52. [60]

    Optimization algorithm for the generation of ONCV pseudopotentials

    Schlipf, M.; Gygi, F. Optimization algorithm for the generation of ONCV pseudopotentials. Comput. Phys. Commun. 2015, 196, 36--44

    2015

  53. [61]

    P.; Burke, K.; Ernzerhof, M

    Perdew, J. P.; Burke, K.; Ernzerhof, M. Generalized gradient approximation made simple. Phys. Rev. Lett. 1996, 77, 3865--3868

    1996

  54. [62]

    E.; Ernzerhof, M

    Heyd, J.; Scuseria, G. E.; Ernzerhof, M. Hybrid functionals based on a screened Coulomb potential. J. Chem. Phys. 2003, 118, 8207--8215

    2003

  55. [63]

    H.; Govoni, M.; Galli, G

    Skone, J. H.; Govoni, M.; Galli, G. Self-consistent hybrid functional for condensed systems. Phys. Rev. B 2014, 89, 195112

    2014

  56. [64]

    pDMET: A code for periodic DMET calculations

    Mitra, A. pDMET: A code for periodic DMET calculations. https://github.com/mitra054/mypDMET, 2022; Accessed July 1, 2023

    2022

  57. [65]

    C.; Blunt, N

    Sun, Q.; Berkelbach, T. C.; Blunt, N. S.; Booth, G. H.; Guo, S.; Li, Z.; Liu, J.; McClain, J. D.; Sayfutyarova, E. R.; Sharma, S.; Wouters, S.; Chan, G. K.-L. PySCF: the Python-based simulations of chemistry framework. WIREs Comput. Mol. Sci. 2018, 8, e1340

    2018

  58. [66]

    Sun, Q. et al. Recent developments in the PySCF program package. J. Chem. Phys. 2020, 153, 024109

    2020

  59. [67]

    Pizzi, G. et al. Wannier90 as a community code: New features and applications. J. Phys. Condens. Mat. 2020, 32, 165902

    2020

  60. [68]

    Pham, H. Q. pyWannier90: A Python interface for wannier90. https://github.com/hungpham2017/pyWannier90, 2019; Accessed July 1, 2023

    2019

  61. [69]

    Separable dual-space Gaussian pseudopotentials

    Goedecker, S.; Teter, M.; Hutter, J. Separable dual-space Gaussian pseudopotentials. Phys. Rev. B 1996, 54, 1703--1710

    1996

  62. [70]

    Gaussian basis sets for accurate calculations on molecular systems in gas and condensed phases

    VandeVondele, J.; Hutter, J. Gaussian basis sets for accurate calculations on molecular systems in gas and condensed phases. J. Chem. Phys. 2007, 127, 114105

    2007

  63. [71]

    A.; Roos, B

    Veryazov, V.; Malmqvist, P. A.; Roos, B. O. How to select active space for multiconfigurational quantum chemistry? Int. J. Quantum Chem. 2011, 111, 3329--3338

    2011

  64. [72]

    J.; Reiher, M

    Stein, C. J.; Reiher, M. Automated selection of active orbital spaces. J. Chem. Theory Comput. 2016, 12, 1760--1771

    2016

  65. [73]

    R.; Sun, Q.; Chan, G

    Sayfutyarova, E. R.; Sun, Q.; Chan, G. K.-L.; Knizia, G. Automated construction of molecular active spaces from atomic valence orbitals. J. Chem. Theory Comput. 2017, 13, 4063--4078

    2017

  66. [74]

    J.; Truhlar, D

    Bao, J. J.; Truhlar, D. G. Automatic active space selection for calculating electronic excitation energies based on high-spin unrestricted Hartree–Fock orbitals. J. Chem. Theory Comput. 2019, 15, 5308--5318

    2019

  67. [75]

    S.; Gagliardi, L

    King, D. S.; Gagliardi, L. A ranked-orbital approach to select active spaces for high-throughput multireference computation. J. Chem. Theory Comput. 2021, 17, 2817--2831

    2021

  68. [76]

    B.; Awschalom, D

    Alkauskas, A.; Buckley, B. B.; Awschalom, D. D.; Van de Walle, C. G. First-principles theory of the luminescence lineshape for the triplet transition in diamond NV centres. New J. Phys. 2014, 16, 073026

    2014

  69. [77]

    o f, Jan and Heiberg, Anders and Roos, Bj\

    Jin, Y.; Govoni, M.; Wolfowicz, G.; Sullivan, S. E.; Heremans, F. J.; Awschalom, D. D.; Galli, G. Photoluminescence spectra of point defects in semiconductors: Validation of first-principles calculations. Phys. Rev. Mater. 2021, 5, 084603 mcitethebibliography achemso-demo.bib0...

    2021

  70. [78]

    Implementation strategies in phonopy and phono3py

    Togo, A.; Chaput, L.; Tadano, T.; Tanaka, I. Implementation strategies in phonopy and phono3py. J. Phys. Condens. Matter 2023, 35, 353001

    2023

  71. [79]

    First-principles phonon calculations with phonopy and phono3py

    Togo, A. First-principles phonon calculations with phonopy and phono3py. J. Phys. Soc. Jpn. 2023, 92, 012001

    2023

  72. [80]

    E.; Heremans, F

    Jin, Y.; Govoni, M.; Wolfowicz, G.; Sullivan, S. E.; Heremans, F. J.; Awschalom, D. D.; Galli, G. Photoluminescence spectra of point defects in semiconductors: Validation of first-principles calculations. Phys. Rev. Mater. 2021, 5, 084603 mcitethebibliography supp-info.tex0000...

    2021

Pith tools

Reviewed August 10, 2026 · model on record in the stance chip above.