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arxiv: 2605.13211 · v2 · pith:WVISALAKnew · submitted 2026-05-13 · ❄️ cond-mat.mes-hall

Highly Efficient Exciton Modulation in MoSe₂/PdSe₂ Heterostructures

Petr Rozhin , Emma Contin , Danae Katrisioti , Till Weickhardt , Muhammad Sufyan Ramzan , Micol Bertolotti , Nouha Loudhaief , Bing Wu
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Zden\v{e}k Sofer Takashi Taniguchi Kenji Watanabe Leonardo Puppulin Stefano Dal Conte Caterina Cocchi Ioannis Paradisanos Giancarlo Soavi Giovanni Antonio Salvatore Domenico De Fazio
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Pith reviewed 2026-05-20 21:42 UTC · model grok-4.3

classification ❄️ cond-mat.mes-hall
keywords exciton modulationvan der Waals heterostructuresMoSe2/PdSe2photoluminescence quantum yieldinterlayer couplingA-exciton enhancementB-exciton quenchingtype-I heterostructure
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The pith

Interlayer electronic coupling in MoSe2/PdSe2 heterostructures redistributes excitons to boost A-exciton emission sixfold.

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

The paper shows that stacking monolayer MoSe2 with PdSe2 in a type-I van der Waals heterostructure creates interlayer electronic coupling. This coupling quenches the higher-energy B-exciton while strongly enhancing emission from the radiative A-exciton at room temperature. The result is a sixfold increase in photoluminescence intensity and a rise in quantum yield from about 1 percent to 6 percent. Measurements across power, temperature, and excitation wavelengths indicate that exciton populations are redirected toward radiative decay paths and that exciton-exciton annihilation is suppressed. The broadband nature of the enhancement suggests this is a general effect of the interface coupling rather than a tuned resonance.

Core claim

In the MoSe₂/PdSe₂ van der Waals heterostructure, interlayer electronic coupling redistributes exciton populations from the B-exciton to the lower-energy radiative A-exciton channel. This results in a pronounced enhancement of room-temperature A-exciton emission by a factor of approximately six, corresponding to a photoluminescence quantum yield of 6% compared to 1% in the isolated monolayer. Power-dependent measurements indicate reduced exciton-exciton annihilation, while temperature-dependent data show a crossover to quenched emission at low temperatures. Broadband photoluminescence excitation spectroscopy confirms the effect spans 450-725 nm, ruling out resonance-specific mechanisms.

What carries the argument

Interlayer electronic coupling in a type-I MoSe2/PdSe2 heterostructure that redistributes exciton populations toward the radiative A-exciton.

If this is right

  • Interlayer coupling provides an efficient route to enhance emission efficiency in two-dimensional semiconductors without chemical modification or applied strain.
  • Suppression of exciton-exciton annihilation occurs as a result of the population redistribution.
  • The enhancement is broadband, applying across excitation wavelengths from 450 to 725 nm.
  • Exciton relaxation pathways can be redirected at the van der Waals interface to favor radiative channels over non-radiative ones.

Where Pith is reading between the lines

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

  • Similar coupling effects might improve performance in other transition metal dichalcogenide heterostructures for light-emitting applications.
  • Interface engineering via such stacks could help overcome defect-related non-radiative losses in practical devices.
  • Device designs could incorporate PdSe2 layers to modulate emission without altering the active MoSe2 material directly.

Load-bearing premise

The measured increase in photoluminescence directly indicates a higher quantum yield from exciton population redistribution rather than from altered absorption, interface defects, or experimental collection efficiency.

What would settle it

Direct measurement of the absorption cross-section in the heterostructure compared to the monolayer MoSe2 to determine if the emission boost matches the absorption change or exceeds it.

Figures

Figures reproduced from arXiv: 2605.13211 by Bing Wu, Caterina Cocchi, Danae Katrisioti, Domenico De Fazio, Emma Contin, Giancarlo Soavi, Giovanni Antonio Salvatore, Ioannis Paradisanos, Kenji Watanabe, Leonardo Puppulin, Micol Bertolotti, Muhammad Sufyan Ramzan, Nouha Loudhaief, Petr Rozhin, Stefano Dal Conte, Takashi Taniguchi, Till Weickhardt, Zden\v{e}k Sofer.

Figure 1
Figure 1. Figure 1: Structural and electronic properties of the MoSe2/PdSe2 heterostructure on an hBN substrate: (a) Optical image of the MoSe2/PdSe2/hBN heterostructure and (b) electronic band structures and projected density of states (PDOS) of a model heterostructure formed by 1L MoSe2 and 4L PdSe2. The vacuum level is set to 0 eV, and the Fermi level is marked with a horizontal dashed line in the mid-gap. The red arrow in… view at source ↗
Figure 2
Figure 2. Figure 2: PL spectra of the 1L region and the HS region (a) A-exciton PL enhancement in the HS region at 514 nm excitation (b) B-exciton quenching in the HS region. PL intensity is reported in arbitrary units (a.u.), corresponding to detector counts. ∼6× relative to the 1L region. Assuming comparable op￾tical absorption at the excitation wavelength and identi￾cal light extraction efficiencies, we estimate an externa… view at source ↗
Figure 3
Figure 3. Figure 3: MoSe2/PdSe2 HS PL mapping a) A-exciton PL intensity map, IA (b) B/A exciton intensity ratio map, IB/IA (a) (a) (b) [PITH_FULL_IMAGE:figures/full_fig_p005_3.png] view at source ↗
Figure 4
Figure 4. Figure 4: Laser power-dependent PL spectra of A-exciton at (a) room temperature and (b) cryogenic temperature. The reported power denotes the incident laser power at the sample. α ≃ 0.71 and α ≃ 0.85, respectively, which is attributed to EEA at high carrier densities [60]. Importantly, unlike the room-temperature behavior, the large PL enhance￾ment disappears at 78 K, with the HS region exhibiting lower intensity th… view at source ↗
Figure 5
Figure 5. Figure 5: Temperature-dependent PL measurements of (a) the 1L region and (b) the HS region (c) Temperature-dependent peak PL measurements of the 1L region and the HS region (d) Temperature dependence of the 1L region and the HS region B-exciton-to-A-exciton intensity ratio. ing [47], which can limit dark–bright exciton conversion and intervalley relaxation [61, 62], thereby reducing the repopulation of the radiative… view at source ↗
Figure 6
Figure 6. Figure 6: (a) PLE spectra of the 1L and the HS (b) PLE intensity ratio between the HS and the 1L. that interfacial band alignment dictates the transition between emission enhancement and suppression. CONCLUSIONS We have shown that interlayer coupling in MoSe2/PdSe2 HSs enables strong enhancement of A-exciton emission in 1L MoSe2, increasing the PLQY from ∼1% in the reference monolayer to 6% at room temperature. Our … view at source ↗
read the original abstract

Controlling exciton recombination in atomically thin semiconductors is central to their optoelectronic functionality, as the competition between radiative and non-radiative decay channels governs emission efficiency. Existing approaches, such as defect passivation, chemical doping, dielectric engineering, and strain tuning, primarily aim to suppress non-radiative losses. Here, we report a pronounced $\sim$6-fold enhancement of room-temperature A-exciton emission in a type-I MoSe$_2$/PdSe$_2$ van der Waals heterostructure, yielding a photoluminescence quantum yield of 6 %, compared to $\sim$1 % for as-exfoliated monolayer MoSe$_2$. This enhancement is accompanied by strong quenching of the B-exciton, consistent with interlayer electronic coupling that redistributes exciton populations toward the radiative A-exciton channel. Power- and temperature-dependent measurements reveal a suppression of exciton-exciton annihilation and a crossover to quenched emission at low temperature, indicating a redistribution of exciton relaxation pathways. Photoluminescence excitation spectroscopy further reveals a broadband enhancement spanning 450-725 nm, ruling out a resonance-specific mechanism. These results demonstrate that interlayer electronic coupling can be used as an efficient means to redirect exciton populations toward radiative channels, enhancing emission efficiency in two-dimensional semiconductors without chemical modification or strain.

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 a ~6-fold enhancement of room-temperature A-exciton photoluminescence in a type-I MoSe2/PdSe2 van der Waals heterostructure, yielding a photoluminescence quantum yield of 6% versus ~1% for as-exfoliated monolayer MoSe2. This is attributed to interlayer electronic coupling that redistributes exciton populations toward the radiative A-exciton channel, accompanied by strong B-exciton quenching. Supporting evidence includes power-dependent suppression of exciton-exciton annihilation, a low-temperature crossover to quenched emission, and broadband photoluminescence excitation enhancement spanning 450-725 nm, ruling out resonance-specific effects.

Significance. If the interpretation that the intensity increase reflects a genuine quantum-yield gain from population redistribution holds, the result would demonstrate an efficient, non-chemical route to enhance radiative efficiency in 2D semiconductors via heterostructure coupling. The multi-probe experimental approach (power, temperature, and excitation-wavelength dependence) adds robustness to the exciton-dynamics picture and could inform design of light-emitting devices based on transition-metal dichalcogenides.

major comments (2)
  1. [Abstract] Abstract: The central claim that the observed ~6-fold A-exciton PL intensity increase corresponds to a true rise in quantum yield (6% vs. ~1%) from interlayer coupling requires that absorption at the excitation energy, out-coupling efficiency, and non-radiative defect rates remain unchanged or are explicitly normalized. No reflectance, absorption, or absolute-QY calibration data against a standard are described, leaving dielectric screening by PdSe2 or interface effects as viable alternative explanations for the intensity change.
  2. [Power- and temperature-dependent measurements] Power- and temperature-dependent measurements section: The reported suppression of exciton-exciton annihilation and the low-temperature crossover are described qualitatively without error bars, raw spectra, or quantitative rate-equation modeling. This weakens the ability to distinguish population redistribution from other mechanisms such as interface passivation or altered annihilation coefficients.
minor comments (1)
  1. [Abstract] The phrase 'as-exfoliated monolayer MoSe2' should specify whether the reference samples experienced identical substrate and processing conditions as the heterostructure to enable direct comparison.

Simulated Author's Rebuttal

2 responses · 0 unresolved

We thank the referee for the careful reading and constructive feedback on our manuscript. The comments have prompted us to strengthen the presentation of the quantum-yield interpretation and the supporting measurements. We address each major comment below and indicate the revisions made.

read point-by-point responses

  1. Referee: [Abstract] Abstract: The central claim that the observed ~6-fold A-exciton PL intensity increase corresponds to a true rise in quantum yield (6% vs. ~1%) from interlayer coupling requires that absorption at the excitation energy, out-coupling efficiency, and non-radiative defect rates remain unchanged or are explicitly normalized. No reflectance, absorption, or absolute-QY calibration data against a standard are described, leaving dielectric screening by PdSe2 or interface effects as viable alternative explanations for the intensity change.

    Authors: We agree that absolute quantum-yield determination requires explicit checks on absorption and collection efficiency. The reported 6% and 1% values are relative estimates obtained by comparing integrated A-exciton PL intensities under identical 532 nm excitation and collection conditions for the monolayer and heterostructure. In the revised manuscript we have added room-temperature reflectance spectra (new Figure S3) demonstrating that absorption at the excitation wavelength differs by less than 10% between the two samples. We have also expanded the discussion to explain why uniform dielectric screening or interface passivation cannot account for the observed selective A-exciton enhancement together with strong B-exciton quenching; these alternatives would affect both resonances similarly. A full absolute-QY calibration against a reference standard was not performed and is noted as a limitation. revision: yes

  2. Referee: [Power- and temperature-dependent measurements] Power- and temperature-dependent measurements section: The reported suppression of exciton-exciton annihilation and the low-temperature crossover are described qualitatively without error bars, raw spectra, or quantitative rate-equation modeling. This weakens the ability to distinguish population redistribution from other mechanisms such as interface passivation or altered annihilation coefficients.

    Authors: We acknowledge that the original presentation was largely qualitative. In the revised version we have added error bars to the power-dependent PL intensity and integrated A-exciton yield plots (revised Figure 3), included representative raw spectra in the supplementary information (new Figure S4), and provided a more detailed discussion of the observed trends. While a complete rate-equation model with fitted parameters is not included, the combination of power-dependent suppression of annihilation, the temperature-induced crossover to quenched emission, and the broadband PLE enhancement collectively supports population redistribution over uniform passivation or simple changes in annihilation rates. We have clarified this reasoning in the text. revision: partial

Circularity Check

0 steps flagged

No circularity: experimental reporting of direct measurements

full rationale

The paper is an experimental study reporting photoluminescence intensity, quantum yield estimates, power- and temperature-dependent data, and PLE spectra in MoSe2/PdSe2 heterostructures. The central claim of ~6-fold A-exciton enhancement and 6% QY (vs ~1% for bare monolayer) is presented as a direct observational result from measurements, not derived from any model, equation, or fitted parameter that loops back to the same dataset. No self-definitional steps, fitted inputs called predictions, or load-bearing self-citations appear in the provided abstract or described content. The work compares heterostructure data to as-exfoliated controls and uses broadband PLE to support the interpretation, remaining self-contained against external benchmarks without reducing claims to internal construction.

Axiom & Free-Parameter Ledger

0 free parameters · 2 axioms · 0 invented entities

The central claim rests on standard assumptions of photoluminescence quantum-yield extraction and on the classification of the heterostructure as type-I. No free parameters or invented entities are introduced in the abstract.

axioms (2)
  • domain assumption Photoluminescence intensity ratios can be converted to absolute quantum yields using reference samples or known collection efficiencies without significant systematic error from interface effects.
    Invoked when the abstract states a 6% quantum yield for the heterostructure versus 1% for monolayer MoSe2.
  • domain assumption The heterostructure is type-I, placing both A and B excitons of MoSe2 inside the PdSe2 gap.
    Stated explicitly in the abstract as the basis for interlayer coupling interpretation.

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