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Origin of C(1s) binding energy shifts in amorphous carbon materials

2025· article· en· W4408851648 on OpenAlexaff
Michael Walter, Filippo Mangolini, J. Brandon McClimon, Robert W. Carpick, Michael Moseler

Bibliographic record

VenuePhysical Review Materials · 2025
Typearticle
Languageen
FieldMaterials Science
TopicDiamond and Carbon-based Materials Research
Canadian institutionsInnovation Cluster (Canada)
FundersH2020 Marie Skłodowska-Curie ActionsDeutsche ForschungsgemeinschaftMarie CurieWelch FoundationNational Science Foundation
KeywordsMaterials scienceAmorphous carbonAmorphous solidCarbon fibersBinding energyEnergy (signal processing)Chemical engineeringChemical physicsCrystallographyComposite materialAtomic physicsComposite number

Abstract

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The quantitative evaluation of the carbon hybridization state by x-ray photoelectron spectroscopy (XPS) has been a surface-analysis problem for the last three decades due to the challenges associated with the unambiguous identification of the characteristic binding energy values for <a:math xmlns:a="http://www.w3.org/1998/Math/MathML"> <a:msup> <a:mrow> <a:mi>sp</a:mi> </a:mrow> <a:mn>2</a:mn> </a:msup> </a:math> - and <b:math xmlns:b="http://www.w3.org/1998/Math/MathML"> <b:msup> <b:mrow> <b:mi>sp</b:mi> </b:mrow> <b:mn>3</b:mn> </b:msup> </b:math> -bonded carbon. Here, we computed the binding energy values of C(1s) core electrons on the absolute energy scale for model structures of amorphous carbon (a-C) using density functional theory (DFT). The DFT calculations show that in the case of hydrogen-free a-C, the C(1s) binding energy for <c:math xmlns:c="http://www.w3.org/1998/Math/MathML"> <c:msup> <c:mrow> <c:mi>sp</c:mi> </c:mrow> <c:mn>3</c:mn> </c:msup> </c:math> carbon atoms is a distribution found approximately 1 eV higher than the binding energy distribution of <d:math xmlns:d="http://www.w3.org/1998/Math/MathML"> <d:msup> <d:mrow> <d:mi>sp</d:mi> </d:mrow> <d:mn>2</d:mn> </d:msup> </d:math> -hybridized carbons. However, the introduction of hydrogen in the a-C network reduces the distance between the characteristic signals of <e:math xmlns:e="http://www.w3.org/1998/Math/MathML"> <e:msup> <e:mrow> <e:mi>sp</e:mi> </e:mrow> <e:mn>3</e:mn> </e:msup> </e:math> - and <f:math xmlns:f="http://www.w3.org/1998/Math/MathML"> <f:msup> <f:mrow> <f:mi>sp</f:mi> </f:mrow> <f:mn>2</f:mn> </f:msup> </f:math> -bonded carbon due to the increased ability to screen the core hole by neighboring hydrogen atoms as compared to carbon atoms. This effect hinders the unambiguous quantification of the carbon hybridization state on the basis of C(1s) XPS data alone. This work can assist surface scientists in the use of XPS for the accurate characterization of carbon-based materials.

Fetched live from OpenAlex and de-inverted. Abstracts are not stored in this database: the inverted indexes are 8.6 GB of the frame’s 9.3 GB of text, and the host has 13 GB free.

How this classification was reachedexpand

Full frame distilled prediction

Teacher imitation

Not calibrated prevalence, not ground truth. Human validation pending. Learned from the 10,348 direct Codex labels and 10,348 direct Gemma labels. Candidate is the union of thresholded teacher heads; consensus is their intersection. These outputs are machine_predicted_unvalidated and are not human labels or direct frontier model labels.

metaresearch head score (Codex)0.002
metaresearch head score (Gemma)0.000
Version: codex-gemma-dda1882f352aValidation status: machine_predicted_unvalidated
Candidate categoriesMeta-epidemiology (narrow), Insufficient payload (model declined to judge)
Consensus categoriesnone
DomainCandidate signal: none · Consensus signal: none
Study designCandidate signal: Bench or experimental · Consensus signal: Bench or experimental
GenreCandidate signal: Empirical · Consensus signal: Empirical
Teacher disagreement score0.007
Threshold uncertainty score1.000

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0020.000
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0020.000
Bibliometrics0.0000.001
Science and technology studies0.0000.000
Scholarly communication0.0000.000
Open science0.0010.000
Research integrity0.0000.000
Insufficient payload (model declined to judge)0.0010.000

Machine scores (provisional)

The two teacher heads of the student model, read on this work. A score orders the frame for review; it never asserts a category, and the validation status ships verbatim with every row.

Baseline scores from an immature model (maturity gate not passed, 7 training rounds). Scores rank; they never assert a category.

Opus teacher head0.019
GPT teacher head0.330
Teacher spread0.312 · how far apart the two teachers sit on this one work
Validation statusscore_only:v0-immature-baseline · verbatim from the scoring run: score_only means the number may rank works, and no category label ships from it

Classification

machine, unvalidated

Machine predicted; a candidate call from one teacher head, not a consensus.

Study designBench or experimental
Domainnot available
GenreEmpirical

How this classification was reached, model by model and score by score, is at the end of the page under "How this classification was reached".

Quick stats

Citations11
Published2025
Admission routes1
Has abstractyes

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