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Fast Interlayer Energy Transfer from the Lower Bandgap MoS2 to the Higher Bandgap WS2

Version 1.0

Gayatri; Mehdi Arfaoui; Debashish Das; Tomasz Kazimierczuk; Sabrine Ayari; Natalia Zawadzka; Takashi Taniguchi; Kenji Watanabe; Adam Babiński; Saroj K. Nayak; Maciej R. Molas; Arka Karmakar, 2026, "Fast Interlayer Energy Transfer from the Lower Bandgap MoS2 to the Higher Bandgap WS2", https://doi.org/10.58132/O4SZ34, Dane Badawcze UW, V1

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Description

This description is related to the article - Fast Interlayer Energy Transfer from the Lower Bandgap MoS2 to the Higher Bandgap WS2


Energy transfer (ET) is a dipole-dipole interaction, mediated by the virtual photon. Traditionally, ET happens from the higher (donor) to lower bandgap (acceptor) material. However, in some rare instances, ET can happen from the lower-to-higher bandgap material, depending on the strong overlap between the acceptor photoluminescence (PL) and the donor absorption spectra. In this work, we report an ET process from the lower bandgap MoS2 to the higher bandgap WS2, due to a near 'resonant' overlap between the MoS2 B and WS2 A excitonic levels. Changing the MoS2 bandgap from direct-to-indirect by increasing the layer number results in a reduced ET rate, evidenced by the quenching of the WS2 PL emission. Our work shows at 300 K, the ET timescale of ~33 fs is faster than the reported thermalization of the MoS2 excitonic intervalley scattering (K to K') time and competing with the ultrafast charge transfer timescale. Thus, allowing us to open a new direction in understanding the competing inter/intralayer processes.

(2026-01-09)
Subject
Physics
Keyword

Förster Type Energy Transfer, Van der Waals heterostructures, 2D material

Related Publication

doi: 10.1038/s41699-026-00661-w

Notes
The differential RC measurements were performed using a tungsten–halogen lamp focused by a Mitutoyo Plan Apo SL 50× (N.A. 0.42) objective. The sample was mounted on a piezo stage with free movements in x-y-z directions. The signal was directed from the sample to the Princeton spectrometer equipped with 150 grooves/mm, and then detected using a CCD camera. The differential RC is defined as (RsRsub)/(Rs+Rsub), where Rs is the reflection intensity from the sample and Rsub is the reflection intensity from the substrate. Absorbance spectra were calculated from the RC data as reported in ref.34,49 Ambient condition μ-PL/PLE experiments were performed using a broadband supercontinuum laser source connected to a monochromator to control the excitation wavelength. The laser beam was focused on the sample using a Mitutoyo Plan Apo SL 50× (N.A. 0.55) objective with spot of about ~1 µm diameter. The average power was kept constant for all the wavelengths only at ~3.6 µW using a noise eater to avoid heating up the sample and any high power induced nonlinear effect. For LT measurement, the sample was loaded into a continuous flow cryostat and cooled down with liquid helium (LHe) flow. The gaps in the PL spectra (Figure 2c) are due to the removal of the transmission line (leakage) from a longpass filter at the detection path (Figure S20). We performed the TR-PL measurements using a S20 synchroscan streak camera. The sample was excited with 450 nm (~2.75 eV) excitation using a second harmonic of a Ti:Sapphire femtosecond oscillator with pulse duration < 200 fs, which operates at a fundamental wavelength of ~900 nm. The average excitation
power was kept at ~26 µW. The experimental data was fitted using a bi-exponential decay function:
𝑦 = 𝑦0 + 𝐴1𝑒𝑥𝑝 (−(𝑥 − 𝑥0)𝑡1) + 𝐴2𝑒𝑥𝑝 (−(𝑥 − 𝑥0)𝑡2)
where, 𝑦0 = offset, 𝑥0 = center, 𝐴1 & 𝐴2 = amplitude, and 𝑡1 & 𝑡2 = time constant (𝑡2 > 𝑡1).
Fitted decaytime constants are as follows,
MoS2 in 1L HS: 𝑡1 = ~10.25 ± 0.71 ps, 𝑡2 = ~28.84 ± 3.05 ps
WS2 in 1L HS : 𝑡1 = ~11.01 ± 0.36 ps, 𝑡2 = ~33.24 ± 1.21 ps
WS2 in 2L HS : 𝑡1 = ~10.73 ± 0.32 ps, 𝑡2 = ~42.40 ± 0.91 ps

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Fig1_a.txt
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Fig. 1(a) Room temperature (RT) absorption spectra of 1Ls MoS2 and WS2, calculated from the RC experiment. Shaded area shows an almost 'resonant' overlap between the MoS2 B (BMo) and WS2 A (AW) excitonic peaks. A constant background was added to WS2 spectrum for a better visual representation. The data composed of 9 columns: 1 Energy (eV); 2 Reflectance from MoS2 (counts); 3 Reflectance from WS2 (counts); 4 Reflectance from Background (hBN) (counts); 5 Reflectance contrast of MoS2 (2-4)/(2+4); 5 Reflectance contrast of WS2 (3-4)/(3+4); 6 Absorbance of MoS2 calculated from reflectance contrast (0.25*((2.75^2)-1)*5); 7 Absorbance of WS2 calculated from reflectance contrast (0.25*((2.75^2)-1)*6); 8 Absorbance of WS2 with constant (7+0.2)
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Fig2_b_1L_HS.txt
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Fig. 2 (b)- 1L HS Photoluminescence excitation (PLE) false colormaps for 1L HS area taken at 300 K. The data is in matrix format (4721 x 76). First row is Excitation energy (eV) and first column is Emission energy (eV).
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Fig2_b_2L_HS.txt
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Fig.2 (b)- 2L HS Photoluminescence excitation (PLE) false colormaps for 2L HS area taken at 300 K. The data is in matrix format (4721 x 76). First row is Excitation energy (eV) and first column is Emission energy (eV).
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Fig2_b_4L_HS.txt
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Fig.2 (b)- 4L HS Photoluminescence excitation (PLE) false colormaps for 4L HS area taken at 300 K. The data is in matrix format (4721 x 76). First row is Excitation energy (eV) and first column is Emission energy (eV).
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Fig2_b_5L_HS.txt
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Fig.2 (b)- 5L HS Photoluminescence excitation (PLE) false colormaps for 5L HS area taken at 300 K. The data is in matrix format (4584 x 76). First row is Excitation energy (eV) and first column is Emission energy (eV).
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Fig2_b_WS2.txt
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Fig.2 (b)- 1L WS2 Photoluminescence excitation (PLE) false colormaps for 1L WS2 area taken at 300 K. The data is in matrix format (4584 x 76). First row is Excitation energy (eV) and first column is Emission energy (eV).
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Fig2_c.txt
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Fig. 2 (c)RT photoluminescence (PL) spectra from all the regions under 2.4 eV laser excitation. Inset shows the MoS2 PL emission. 1L HS area shows ~3× brighter PL emission as compared to the isolated WS2 region. The data composed of 9 columns: 1 Energy (eV); 2 PL intensity from WS2 region (counts); 3 PL intensity from MoS2 region (counts); 4 PL intensity from 1L HS region (counts); 5 PL intensity from 2L HS region (counts); 6 PL intensity from 4L HS region (counts); 7 PL intensity from 5L HS region (counts).
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Fig2_d.txt
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Fig. 2 (d) PL enhancement factor as a function of the excitation energy calculated from the PLE maps shown in (b). To calculate the enhancement factor, PL intensities from the HS areas are divided by the WS2 emission (along the vertical dashed line in (b)). 1L HS area shows an increasing PL emission with the excitation energy and the 2L HS area shows a similar behavior after ~2.17 eV excitation. While, the 4L and 5L HS areas show PL quenching throughout the entire excitation energy. The data composed of 10 columns: 1 Energy (eV); 2 PL intensity of WS2 region at emission energy 2eV; 3 PL intensity of 1L HS region at emission energy 2eV; 4 PL intensity of 2L HS region at emission energy 2eV; 5 PL intensity of 4L HS region at emission energy 2eV; 6 PL intensity of 5L HS region at emission energy 2eV 7 PL enhancement factor for 1L HS; 8 PL enhancement factor for 2L HS; 9 PL enhancement factor for 4L HS; 10 PL enhancement factor for 5L HS.
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Fig2_e.txt
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Fig. 2 (e) Low temperature (LT) (5 K) PL spectra from all the regions under 2.4 eV excitation energy. WS2 neutral exciton (X0) shows a slight enhancement only in the 1L HS area (marked by the shaded region). To differentiate the emissions from the individual regions a similar color scheme is used as in (c). The data composed of 6 columns: 1 Energy (eV); 2 PL intensity from WS2 region (counts); 3 PL intensity from 1L HS region (counts); 4 PL intensity from 2L HS region (counts); 5 PL intensity from 4L HS region (counts); 6 PL intensity from 5L HS region (counts).
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Fig3.txt
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Fig. 3 The squared transition dipole moments (TDM) at K valley is plotted along with the energy difference between the corresponding bands of 1L to 5L MoS2 and 1L WS2, respectively. Red and black bars correspondingly represent the A and B excitonic transitions. The data composed of 12 columns: 1 Energy for 1L MoS2 (eV); 2 TDM (Debye^2) for 1L MoS2; 3 Energy for 2L MoS2 (eV); 4 TDM (Debye^2) for 2L MoS2; 5 Energy for 3L MoS2 (eV); 6 TDM (Debye^2) for 3L MoS2; 7 Energy for 4L MoS2 (eV); 8 TDM (Debye^2) for 4L MoS2; 9 Energy for 5L MoS2 (eV); 10 TDM (Debye^2) for 5L MoS2; 11 Energy for 1L WS2 (eV); 12 TDM (Debye^2) for 1L WS2
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