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arxiv: 2605.22932 · v1 · pith:5HZ253MEnew · submitted 2026-05-21 · ❄️ cond-mat.mtrl-sci

Thickness-Dependent Spintronic Terahertz Emission in MBE-Grown PtTe₂: From Semiconductor to Type-II Dirac Semimetal

Rahul Sharma , Sylvain Massabeau , Armando Pezo , Ekta Yadav , Viliam Vreten\'ar , Ravi K. Biroju , Fatima Ibrahim , Sukhdeep Dhillon
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Alain Marty Isabelle Gomes de Moraes Adrien Michon Jing Li Mairbek Chshiev Henri Jaffr\`es Jean-Marie George Matthieu Jamet
This is my paper

Pith reviewed 2026-05-25 05:41 UTC · model grok-4.3

classification ❄️ cond-mat.mtrl-sci
keywords PtTe2spintronic THz emissiontype-II Dirac semimetalthickness dependencetopological surface statesRashba splittingMBE growthspin-to-charge conversion
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The pith

Spintronic THz emission in PtTe2 is absent in the single-layer semiconductor phase, activates at the 2 ML semimetal transition, and reaches six times the amplitude of a platinum reference at 10 ML before declining due to reabsorption.

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

The paper demonstrates that spintronic terahertz emission in MBE-grown PtTe2 films follows the material's thickness-driven change from semiconductor to type-II Dirac semimetal. Emission vanishes in the 1 ML semiconducting state, switches on sharply near 2 ML as the semimetallic phase appears, maximizes at six times a Pt reference at 10 ML, and falls at greater thicknesses because the thicker metallic film reabsorbs the THz radiation. The non-monotonic dependence is attributed to multi-channel spin-to-charge conversion that strengthens with the development of topological surface states and interfacial Rashba splitting. First-principles calculations of interfacial spin accumulation match the measured trend, supporting the picture over a conventional bulk inverse spin Hall process alone.

Core claim

In PtTe2 the spintronic THz emission tracks the underlying electronic phase diagram directly: it is absent in the single-layer semiconducting phase, turns on sharply at the semimetal transition near 2 ML, and reaches a peak amplitude six times that of an equivalent Pt reference at 10 ML, before declining at larger thicknesses due to THz reabsorption in the increasingly metallic film. This behavior reflects a multi-channel spin-to-charge conversion process in which spin-momentum-locked topological surface states and a thickness-dependent interfacial Rashba splitting both contribute and strengthen as the type-II Dirac band structure develops, as confirmed by first-principles calculations ofthe

What carries the argument

Thickness-driven transition from semiconductor to type-II Dirac semimetal that activates multi-channel spin-to-charge conversion through topological surface states and interfacial Rashba splitting.

If this is right

  • Thickness can be used as a control knob to optimize spintronic THz emitter output beyond the fixed spin Hall conductivity limit of any single material.
  • The same thickness engineering applies to spin-orbit torque performance in SOT-MRAM devices.
  • The approach extends to the broader class of dimensionally tunable topological van der Waals materials.
  • MBE growth with monolayer precision enables reproducible access to the optimal thickness window before reabsorption dominates.

Where Pith is reading between the lines

These are editorial extensions of the paper, not claims the author makes directly.

  • The optimal thickness window identified here could guide device design in other transition-metal dichalcogenides that undergo similar semiconductor-to-semimetal transitions.
  • THz emission itself might serve as a contactless probe of the electronic phase boundary in related layered materials.
  • Integration of these films with existing spintronic stacks could yield compact, broadband THz sources whose output is set by growth parameters rather than material choice alone.

Load-bearing premise

The observed non-monotonic thickness dependence of THz emission arises specifically from the growth of topological surface states and interfacial Rashba splitting rather than from changes in spin injection efficiency or film quality.

What would settle it

Repeating the THz emission measurements while holding the PtTe2 thickness fixed but deliberately altering interface quality or the ferromagnetic injector layer to change spin injection efficiency and checking whether the sharp onset at 2 ML and peak at 10 ML remain unchanged.

Figures

Figures reproduced from arXiv: 2605.22932 by Adrien Michon, Alain Marty, Armando Pezo, Ekta Yadav, Fatima Ibrahim, Henri Jaffr\`es, Isabelle Gomes de Moraes, Jean-Marie George, Jing Li, Mairbek Chshiev, Matthieu Jamet, Rahul Sharma, Ravi K. Biroju, Sukhdeep Dhillon, Sylvain Massabeau, Viliam Vreten\'ar.

Figure 1
Figure 1. Figure 1: Structural and morphological characterization of MBE-grown 1T-PtTe2 thin films. (a) Top and side views of the crystal structure of 1T-PtTe2. Grey (orange) atoms : Pt (Te) atoms (b) Reflection high-energy electron diffraction (RHEED) patterns recorded along the (100) and (110) azimuths of the Gr/SiC substrate (top) and of the PtTe2 monolayer grown on top of the substrate (bottom), confirming epitaxial growt… view at source ↗
Figure 2
Figure 2. Figure 2: PtTe2 THz emission properties. (a) THz emission time traces for Al(3 nm)/Co(3 nm)/PtTe2(10 ML) (blue) compared with the reference sample Al(3 nm)/Co(3 nm)/Pt(1 nm) (red) with equivalent Pt thickness, for small (∼20 mT) in￾plane positive (+B) and negative (−B) magnetic fields. The 10 ML PtTe2 stack has the same conversion sign as Pt and exhibits a sixfold increase in emitted THz electric field compared to t… view at source ↗
Figure 3
Figure 3. Figure 3: Thickness dependence of THz emission. (a) Peak-to-peak amplitude of THz emission from Al/Co/PtTe2 as a function of PtTe2 thickness expressed in monolayer number. (b) Peak-to-peak amplitude of THz emission from Al/Co/Pt as a function of Pt thickness (red dots). The black solid line corresponds to the ISHE fit using equation (1), yielding a spin relaxation length of 0.95 nm. (c) Comparison between THz emissi… view at source ↗
Figure 4
Figure 4. Figure 4: Calculated electronic structure and spin-to-charge conversion in PtTe2 (a) DFT-calculated spin-resolved band structures of PtTe2 slabs at representative thicknesses of 3 ML (i), 6 ML (ii), and 9 ML (iii), plotted along the M–Γ–M high-symmetry direction. The color scale indicates the expectation value of the spin operator ⟨sy⟩ in units of h¯, revealing the progressive development of spin-split bands and top… view at source ↗
read the original abstract

Spintronic terahertz (THz) emitters have established themselves as among the most practical broadband THz sources available, yet their performance remains fundamentally limited by the spin Hall conductivity of the nonmagnetic conversion layer - a quantity that is fixed once the material is chosen. Here, we demonstrate that in PtTe$_2$, a type-II Dirac semimetal within the transition metal dichalcogenide family, this limitation can be circumvented by exploiting the dramatic thickness-driven electronic phase evolution of the material itself. Using molecular beam epitaxy to grow PtTe$_2$ films with single-monolayer precision from 1 to 20 ML, we show that the spintronic THz emission tracks the underlying electronic phase diagram directly: it is absent in the single-layer semiconducting phase, turns on sharply at the semimetal transition near 2 ML, and reaches a peak amplitude six times that of an equivalent Pt reference at 10 ML, before declining at larger thicknesses due to THz reabsorption in the increasingly metallic film. This non-monotonic behavior is inconsistent with a bulk inverse spin Hall mechanism and instead reflects a multi-channel spin-to-charge conversion process in which spin-momentum-locked topological surface states and a thickness-dependent interfacial Rashba splitting both contribute and strengthen as the type-II Dirac band structure develops. First-principles calculations of the interfacial spin accumulation reproduce the experimental trend quantitatively, confirming this physical picture. These findings introduce thickness engineering of van der Waals semimetals as a new and accessible route to optimizing spintronic THz emitters and spin-orbit torques in magnetic memories (SOT-MRAMs), with direct implications for the broader class of dimensionally tunable topological materials.

Editorial analysis

A structured set of objections, weighed in public.

Desk editor's note, referee report, simulated authors' rebuttal, and a circularity audit. Tearing a paper down is the easy half of reading it; the pith above is the substance, this is the friction.

Referee Report

2 major / 1 minor

Summary. The manuscript reports MBE growth of PtTe2 films from 1-20 ML with monolayer precision and measures their spintronic THz emission. It claims the emission is absent in the 1 ML semiconducting phase, turns on sharply near the 2 ML semimetal transition, reaches a peak amplitude six times that of an equivalent Pt reference at 10 ML, and declines at larger thicknesses due to reabsorption. This non-monotonic thickness dependence is attributed to multi-channel spin-to-charge conversion involving developing type-II Dirac topological surface states and thickness-dependent interfacial Rashba splitting, rather than bulk inverse spin Hall effect. First-principles calculations of interfacial spin accumulation are stated to reproduce the experimental trend quantitatively.

Significance. If the central attribution to the electronic phase diagram holds after controls for alternatives, the work demonstrates thickness engineering of van der Waals semimetals as a route to exceed the fixed spin-Hall-conductivity limit of conventional spintronic THz emitters, with potential implications for SOT-MRAM optimization. The monolayer-precision MBE growth and quantitative DFT reproduction are notable strengths that would strengthen the result if paired with fuller experimental documentation.

major comments (2)
  1. [Abstract] Abstract: The central claim of a factor-of-six peak amplitude relative to Pt, together with the non-monotonic thickness series, is presented without raw data, error bars, sample statistics, or explicit controls for film quality, crystallinity, defect density, or interface oxidation. These omissions make it impossible to assess whether the observed trend is robust or could arise from thickness-dependent spin-injection efficiency or measurement artifacts.
  2. [Abstract] Abstract and calculations section: The manuscript states that first-principles interfacial spin accumulation calculations reproduce the trend quantitatively and support the multi-channel (topological surface state + Rashba) interpretation. However, no explicit description is given of how the bulk ISHE contribution is held fixed while only the topological channels are varied; without this, the mapping from phase diagram to emission amplitude remains under-constrained relative to alternative explanations such as conductivity mismatch or interface transparency changes.
minor comments (1)
  1. [Abstract] The abstract refers to 'an equivalent Pt reference' without specifying whether the Pt film thickness, growth method, or measurement geometry are matched to the PtTe2 series.

Simulated Author's Rebuttal

2 responses · 0 unresolved

We thank the referee for their careful reading of the manuscript and for highlighting points that can improve clarity. We provide point-by-point responses to the major comments below.

read point-by-point responses

  1. Referee: [Abstract] Abstract: The central claim of a factor-of-six peak amplitude relative to Pt, together with the non-monotonic thickness series, is presented without raw data, error bars, sample statistics, or explicit controls for film quality, crystallinity, defect density, or interface oxidation. These omissions make it impossible to assess whether the observed trend is robust or could arise from thickness-dependent spin-injection efficiency or measurement artifacts.

    Authors: The abstract is a concise summary; the full manuscript (Sections 3 and 4, Figures 2–4, and Supplementary Information) presents the raw thickness series, error bars derived from multiple independent samples, statistics on film quality via RHEED, AFM, and XRD, and controls for oxidation and crystallinity. To address the concern directly, we will add one sentence to the abstract referencing the statistical robustness of the data set. revision: yes

  2. Referee: [Abstract] Abstract and calculations section: The manuscript states that first-principles interfacial spin accumulation calculations reproduce the trend quantitatively and support the multi-channel (topological surface state + Rashba) interpretation. However, no explicit description is given of how the bulk ISHE contribution is held fixed while only the topological channels are varied; without this, the mapping from phase diagram to emission amplitude remains under-constrained relative to alternative explanations such as conductivity mismatch or interface transparency changes.

    Authors: We agree that the computational section would benefit from greater transparency. In the revised manuscript we will expand the calculations section to detail how the bulk ISHE term is held fixed (using the thickness-independent spin Hall conductivity of the PtTe2 interior) while the interfacial spin accumulation from topological surface states and Rashba splitting is varied with thickness according to the DFT band-structure evolution. This will include the explicit parameters and assumptions used, allowing direct comparison with alternatives such as conductivity mismatch. revision: yes

Circularity Check

0 steps flagged

No significant circularity; experimental series and standard DFT inputs remain independent

full rationale

The paper presents thickness-dependent THz emission data from MBE-grown PtTe2 films (1-20 ML) and compares it to first-principles interfacial spin accumulation calculations whose inputs are standard electronic-structure parameters. No equation or claim reduces a 'prediction' to a parameter fitted against the THz amplitudes themselves, nor does any load-bearing step rely on self-citation for uniqueness or smuggle an ansatz. The non-monotonic trend is shown to deviate from a simple bulk ISHE model via direct experiment, with the multi-channel interpretation offered as a consistent physical picture rather than a definitional tautology. This is the normal case of an experimentally anchored study whose central mapping does not collapse by construction.

Axiom & Free-Parameter Ledger

0 free parameters · 2 axioms · 0 invented entities

The central claim rests on the assumption that MBE-grown PtTe2 films undergo a clean semiconductor-to-type-II Dirac semimetal transition at ~2 ML and that the THz signal is generated by spin-to-charge conversion in the film rather than by extrinsic interface effects. No free parameters are introduced in the abstract. No new entities are postulated.

axioms (2)
  • domain assumption MBE growth produces atomically flat, phase-pure PtTe2 films whose electronic structure evolves with thickness exactly as predicted by prior band-structure calculations
    Invoked to link observed THz amplitude directly to the semiconductor-semimetal transition
  • domain assumption THz emission amplitude is proportional to the spin-to-charge conversion efficiency inside the PtTe2 layer
    Required to interpret the thickness series as evidence for multi-channel conversion rather than changes in spin injection or detection

pith-pipeline@v0.9.0 · 5917 in / 1570 out tokens · 17723 ms · 2026-05-25T05:41:25.241608+00:00 · methodology

discussion (0)

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