{"id":250371,"date":"2025-11-08T01:34:22","date_gmt":"2025-11-08T01:34:22","guid":{"rendered":"https:\/\/www.newsbeep.com\/uk\/250371\/"},"modified":"2025-11-08T01:34:22","modified_gmt":"2025-11-08T01:34:22","slug":"quantum-interference-and-occupation-control-in-high-harmonic-generation-from-monolayer-ws2","status":"publish","type":"post","link":"https:\/\/www.newsbeep.com\/uk\/250371\/","title":{"rendered":"Quantum interference and occupation control in high harmonic generation from monolayer WS2"},"content":{"rendered":"<p>Transition from perturbative to strong-field driven HHG in monolayer WS2<\/p>\n<p>Figure\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"figure anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#Fig1\" rel=\"nofollow noopener\" target=\"_blank\">1a<\/a> schematically illustrates the electronic processes in monolayer WS2 initiated under intense laser driving. In the perturbative regime, nonlinear optical processes primarily arise from excitonic multiphoton transitions at the band gaps located at the K and K\u2032 valleys. Under intense laser fields, excitons become substantially delocalized through hybridization with higher excitonic bound states and continuum states<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 36\" title=\"Kobayashi, Y. et al. Floquet engineering of strongly driven excitons in monolayer tungsten disulfide. Nat. Phys. &#010;                  https:\/\/doi.org\/10.1038\/s41567-022-01849-9&#010;                  &#010;                 (2023).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#ref-CR36\" id=\"ref-link-section-d78054503e948\" rel=\"nofollow noopener\" target=\"_blank\">36<\/a>. Eventually, ionized electrons and holes are driven far beyond the K and K\u2032 valleys over wide regions of momentum space, which opens additional pathways for higher-order nonlinear optical processes via intraband and interband transitions.<\/p>\n<p>Fig. 1: Non-perturbative response of lightwave-driven electron-hole pairs in monolayer WS\u2082.<a class=\"c-article-section__figure-link\" data-test=\"img-link\" data-track=\"click\" data-track-label=\"image\" data-track-action=\"view figure\" href=\"https:\/\/www.nature.com\/articles\/s41467-025-65725-9\/figures\/1\" rel=\"nofollow noopener\" target=\"_blank\"><img decoding=\"async\" aria-describedby=\"Fig1\" src=\"https:\/\/www.newsbeep.com\/uk\/wp-content\/uploads\/2025\/11\/41467_2025_65725_Fig1_HTML.png\" alt=\"figure 1\" loading=\"lazy\" width=\"685\" height=\"605\"\/><\/a><\/p>\n<p>a Illustration of the electronic processes under strong laser excitation: Intense laser driving excites carriers throughout the BZ, and drives them in the respective bands. Interband recombination and intraband currents (red and gray arrows, respectively) emit HHG from various points in the BZ, including beyond K\/K\u2019 valleys. In inset is an illustration of an electrons and holes driven by laser fields. b Experimentally measured HHG spectra as a function of laser intensity from 80 to 350\u2009GW\/cm\u00b2. Note that harmonic yield in (b) is plotted in a logarithmic scale. The spectra display markedly different profiles in the perturbative and non-perturbative regimes, showing onset of HHG plateau at higher driving, and the resonant 7th harmonic appearing in much lower intensities. c Line-cuts of HHG spectra from (b). d Photoluminescence spectra showing clear excitonic signatures with 1\u2009s exciton resonance at 2\u2009eV. e Reflection contrast spectrum indicating absorption near 2\u2009eV, associated with the 1\u2009s exciton resonance. f Measured integrated 7th harmonic yield as a function of laser intensity (obtained from (b)), showing a kink feature arising for both zigzag and armchair orientations. Note that (f) is plotted in a logarithmic scale.<\/p>\n<p>We fabricate large-area, high-quality, WS2 monolayers using a gold-assisted exfoliation method<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 37\" title=\"Liu, F. et al. Disassembling 2D van der Waals crystals into macroscopic monolayers and reassembling into artificial lattices. Science 367, 903&#x2013;906 (2020).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#ref-CR37\" id=\"ref-link-section-d78054503e1007\" rel=\"nofollow noopener\" target=\"_blank\">37<\/a>. To further reduce external defects, the exfoliated monolayer WS2 is encapsulated with hexagonal boron nitride on sapphire substrates via a dry transfer process<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 38\" title=\"Wang, L. et al. One-dimensional electrical contact to a two-dimensional material. Science 342, 614&#x2013;617 (2013).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#ref-CR38\" id=\"ref-link-section-d78054503e1013\" rel=\"nofollow noopener\" target=\"_blank\">38<\/a>. Our home-built femtosecond laser system provides linearly-polarized, mid-infrared pulses with ~ 120\u2009fs duration at 100\u2009kHz repetition rate. We intentionally set the photon energy at ~ 0.28\u2009eV (4500\u2009nm) to match the 7-photon resonant exciton transition at the band edge. The laser power and polarization are precisely controlled and analyzed using polarization optics. HHG spectra are recorded with an electron-multiplying charge-coupled device to achieve a high signal-to-noise ratio. Owing to the combined advantages of high sample quality and high repetition rate, we can sensitively observe the quantum interference features from the perturbative to the non-perturbative regimes, as will be shown below. Additional details on sample preparation, laser setup, and a comparison of HHG spectra with and without hBN encapsulation are provided in the\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#MOESM1\" rel=\"nofollow noopener\" target=\"_blank\">Supplementary Information (SI)<\/a>.<\/p>\n<p>We now investigate HHG in monolayer WS2 as a function the driving intensity. HHG signals are collected and integrated for both parallel and cross-polarization components with respect to the driving laser fields. HHG spectra exhibit markedly different profiles depending on the laser intensity (see Fig.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"figure anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#Fig1\" rel=\"nofollow noopener\" target=\"_blank\">1b, c<\/a>). At ~ 110\u2009GW\/cm2 (red solid line in Fig.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"figure anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#Fig1\" rel=\"nofollow noopener\" target=\"_blank\">1c<\/a>), strong 7th harmonic signals are observed at 1.93\u2009eV, while all other harmonic orders\u2014including lower harmonic orders\u2014are nearly absent. This selective enhancement arises from excitonic resonances at the K and K\u2019 valleys. The reflection contrast spectrum (Fig.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"figure anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#Fig1\" rel=\"nofollow noopener\" target=\"_blank\">1e<\/a>) and HHG spectrum (Fig.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"figure anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#Fig1\" rel=\"nofollow noopener\" target=\"_blank\">1d<\/a>) show absorption and photoluminescence peaks at 2\u2009eV, respectively, originating from 1\u2009s exciton resonances at the optical gap. The 7th harmonic signal is located near 1\u2009s exciton resonances with a small detuning of 70\u2009meV. Up to ~185\u2009GW\/cm2 laser driving, the yield of 7th harmonic in Fig.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"figure anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#Fig1\" rel=\"nofollow noopener\" target=\"_blank\">1f<\/a> scale as \u221d I 7 with respect to laser peak intensity (I). A similar intensity dependence is observed for photoluminescence under mid-infrared laser excitation (see\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#MOESM1\" rel=\"nofollow noopener\" target=\"_blank\">SI<\/a>), indicating that all optical processes observed in this regime are primarily mediated by the 7-photon transitions to the resonant excitonic state. Such excitonic enhancement has been experimentally reported for second harmonic generation in TMD monolayers and heterostructures<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 39\" title=\"Wang, G. et al. Giant enhancement of the optical second-harmonic emission of \\mathrmwse_2 monolayers by laser excitation at exciton resonances. Phys. Rev. Lett. 114, 097403 (2015).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#ref-CR39\" id=\"ref-link-section-d78054503e1050\" rel=\"nofollow noopener\" target=\"_blank\">39<\/a>,<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 40\" title=\"Shree, S. et al. Interlayer exciton mediated second harmonic generation in bilayer MoS2. Nature. Communications 12, 6894 (2021).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#ref-CR40\" id=\"ref-link-section-d78054503e1053\" rel=\"nofollow noopener\" target=\"_blank\">40<\/a>. Recent theoretical studies predict that excitonic resonances can also strongly enhance high-order harmonic generation<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 26\" title=\"Molinero, E. B. et al. Subcycle dynamics of excitons under strong laser fields. Sci. Adv. 10, eadn6985 (2024).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#ref-CR26\" id=\"ref-link-section-d78054503e1058\" rel=\"nofollow noopener\" target=\"_blank\">26<\/a>,<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 36\" title=\"Kobayashi, Y. et al. Floquet engineering of strongly driven excitons in monolayer tungsten disulfide. Nat. Phys. &#010;                  https:\/\/doi.org\/10.1038\/s41567-022-01849-9&#010;                  &#010;                 (2023).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#ref-CR36\" id=\"ref-link-section-d78054503e1061\" rel=\"nofollow noopener\" target=\"_blank\">36<\/a>,<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 41\" title=\"Jensen, S. V. B., Madsen, L. B., Rubio, A. &amp; Tancogne-Dejean, N. High-harmonic spectroscopy of strongly bound excitons in solids. Phys. Rev. A 109, 063104 (2024).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#ref-CR41\" id=\"ref-link-section-d78054503e1064\" rel=\"nofollow noopener\" target=\"_blank\">41<\/a>,<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 42\" title=\"Chang Lee, V., Yue, L., Gaarde, M. B., Chan, Y. &amp; Qiu, D. Y. Many-body enhancement of high-harmonic generation in monolayer MoS2. Nature. Communications 15, 6228 (2024).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#ref-CR42\" id=\"ref-link-section-d78054503e1067\" rel=\"nofollow noopener\" target=\"_blank\">42<\/a>, in agreement with our experimental observations. At higher driving intensity (\u2009&gt;185\u2009GW\/cm2), an HHG plateau spanning 5\u201311th harmonics emerges (Fig.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"figure anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#Fig1\" rel=\"nofollow noopener\" target=\"_blank\">1b, c<\/a>). Under these conditions, the HHG yield becomes non-perturbative, including for the 7th harmonic\u2014the main observable analyzed in this study. Notably, Fig.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"figure anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#Fig1\" rel=\"nofollow noopener\" target=\"_blank\">1f<\/a> reveals a pronounced kink at ~200\u2009GW\/cm2, which is not expected from the perturbative response, and which we will analyze with theory later on.<\/p>\n<p>The crystal orientation dependence of the 7th harmonic yield also indicates the transition from the perturbative to the non-perturbative regime. Figure\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"figure anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#Fig2\" rel=\"nofollow noopener\" target=\"_blank\">2b\u2013f<\/a> present the integrated yield as a function of the angle between the laser field and the WS2 zigzag direction (see the illustration in Fig.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"figure anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#Fig2\" rel=\"nofollow noopener\" target=\"_blank\">2a<\/a>). The crystal axis of WS2 is determined from polarization analysis on even order harmonics (see\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#MOESM1\" rel=\"nofollow noopener\" target=\"_blank\">SI<\/a>). Polarization analysis confirms that the 7th harmonic is absent for the polarization component perpendicular to the driving laser field, as expected from HHG dynamical mirror-symmetry selection rules<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 20\" title=\"Yoshikawa, N. et al. Interband resonant high-harmonic generation by valley polarized electron&#x2013;hole pairs. Nat. Commun. 10, 3709 (2019).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#ref-CR20\" id=\"ref-link-section-d78054503e1098\" rel=\"nofollow noopener\" target=\"_blank\">20<\/a>,<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 43\" title=\"Shen, Y. R. The Principles of Nonlinear Optics. (Wiley, 2003).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#ref-CR43\" id=\"ref-link-section-d78054503e1101\" rel=\"nofollow noopener\" target=\"_blank\">43<\/a> (see\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#MOESM1\" rel=\"nofollow noopener\" target=\"_blank\">SI<\/a>). At a laser intensity of ~ 125\u2009GW\/cm\u00b2, dominated by the perturbative response from excitonic resonances, no apparent dependence on crystal orientation is observed (i.e., an isotropic response). However, in the non-perturbative regime, harmonic signals exhibit strong 60\u00b0 periodic modulation, which becomes increasingly pronounced as the laser intensity rises from ~ 235 to 380\u2009GW\/cm\u00b2, accompanied by significant changes in modulation depth and phase (with 60o periodicity, as expected from crystal symmetry<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 44\" title=\"Neufeld, O., Podolsky, D. &amp; Cohen, O. Floquet group theory and its application to selection rules in harmonic generation. Nat. Commun. 10, 405 (2019).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#ref-CR44\" id=\"ref-link-section-d78054503e1110\" rel=\"nofollow noopener\" target=\"_blank\">44<\/a>) \u2013 Initially, polar plots show stronger harmonic yields along the armchair direction, but as the laser intensity increases the polar plot rotates by 30\u00b0, revealing stronger yields along the zigzag direction. Figure\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"figure anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#Fig2\" rel=\"nofollow noopener\" target=\"_blank\">2f<\/a> is consistent with previous works<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 20\" title=\"Yoshikawa, N. et al. Interband resonant high-harmonic generation by valley polarized electron&#x2013;hole pairs. Nat. Commun. 10, 3709 (2019).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#ref-CR20\" id=\"ref-link-section-d78054503e1117\" rel=\"nofollow noopener\" target=\"_blank\">20<\/a>,<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 21\" title=\"Liu, H. et al. High-harmonic generation from an atomically thin semiconductor. Nat. Phys. 13, 262&#x2013;265 (2017).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#ref-CR21\" id=\"ref-link-section-d78054503e1120\" rel=\"nofollow noopener\" target=\"_blank\">21<\/a> in extreme laser intensities (&gt;1\u2009TW\/cm2). The systematic modification of polar plots is indicative of a change in laser excitation regime, and potentially also the physical mechanisms dominating HHG, as will be discussed below.<\/p>\n<p>Fig. 2: Crystal orientation dependence of the 7th harmonic generation yield.<a class=\"c-article-section__figure-link\" data-test=\"img-link\" data-track=\"click\" data-track-label=\"image\" data-track-action=\"view figure\" href=\"https:\/\/www.nature.com\/articles\/s41467-025-65725-9\/figures\/2\" rel=\"nofollow noopener\" target=\"_blank\"><img decoding=\"async\" aria-describedby=\"Fig2\" src=\"https:\/\/www.newsbeep.com\/uk\/wp-content\/uploads\/2025\/11\/41467_2025_65725_Fig2_HTML.png\" alt=\"figure 2\" loading=\"lazy\" width=\"685\" height=\"454\"\/><\/a><\/p>\n<p>a Schematic of the monolayer WS\u2082 crystal structure and laser polarization axis (red arrow). The x(y)-axis corresponds to the zigzag (armchair) directions, respectively. The angle \u03b8 represents the counterclockwise rotation of the excitation laser polarization relative to the zigzag axis. b\u2013f Crystal orientation dependence of seventh harmonics at increasing laser peak intensities: b 125\u2009GW\/cm\u00b2, c 235\u2009GW\/cm\u00b2, d 305\u2009GW\/cm\u00b2, e 350\u2009GW\/cm\u00b2, and f 380\u2009GW\/cm\u00b2. For low driving power the harmonic response is isotropic and perturbative. At higher intensity in the transition to non-perturbative HHG, a distinct six-fold pattern emerges with emission along the armchair direction. At yet higher intensity the six-fold pattern is slightly less pronounced and rotated by 30\u00b0, exhibiting stronger harmonic intensity along the zigzag direction. The harmonic signals in (b), (c), (d), and (e) are magnified by factors of 200, 10, 2, and 1.3, respectively, to clearly visualize the pattern evolution at lower laser intensities.<\/p>\n<p>Laser intensity-dependent quantum interference in the 7th harmonic spectra<\/p>\n<p>Figure\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"figure anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#Fig3\" rel=\"nofollow noopener\" target=\"_blank\">3c<\/a> presents a 2D color map of high-spectral-resolution 7th harmonic spectra from monolayer WS2 driven in the zig-zag direction as a function of laser intensity (nearly identical spectra are observed along the armchair direction, see\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#MOESM1\" rel=\"nofollow noopener\" target=\"_blank\">SI<\/a>). There are three key surprising results here, which form the main findings of this letter: (i) At ~ 150\u2009GW\/cm\u00b2 where non-perturbative responses emerge from the laser-field-driven carriers, a very significant peak broadening arises. (ii) At slightly higher powers (\u2009~200\u2009GW\/cm2) multiple distinct peaks emerge from the sharp peak that is characteristic of lower intensity driving. At yet higher intensities, ~250\u2009GW\/cm\u00b2, these split peaks converge, resulting in a broader recombined spectral profile. (iii) This evolution is accompanied by a notable kink in the integrated yield of the 7th harmonic (see Fig.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"figure anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#Fig1\" rel=\"nofollow noopener\" target=\"_blank\">1f<\/a> and Fig.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"figure anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#Fig3\" rel=\"nofollow noopener\" target=\"_blank\">3a<\/a>) over the same laser intensity range, whereby the yield does not increase with increasing driving intensity.<\/p>\n<p>Fig. 3: Quantum interference in harmonic generation.<a class=\"c-article-section__figure-link\" data-test=\"img-link\" data-track=\"click\" data-track-label=\"image\" data-track-action=\"view figure\" href=\"https:\/\/www.nature.com\/articles\/s41467-025-65725-9\/figures\/3\" rel=\"nofollow noopener\" target=\"_blank\"><img decoding=\"async\" aria-describedby=\"Fig3\" src=\"https:\/\/www.newsbeep.com\/uk\/wp-content\/uploads\/2025\/11\/41467_2025_65725_Fig3_HTML.png\" alt=\"figure 3\" loading=\"lazy\" width=\"685\" height=\"702\"\/><\/a><\/p>\n<p>a The 7th harmonic yield vs. peak intensity in the zigzag direction (same as Fig.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"figure anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#Fig1\" rel=\"nofollow noopener\" target=\"_blank\">1(f)<\/a>). b Theoretical calculation of the 7th harmonic yield vs. peak intensity under laser excitation along the zigzag direction. We use a pulse duration of ~200\u2009fs to resolve the peak splitting in (f). We confirm that nearly the same behavior is observed for a pulse duration of ~120\u2009fs, corresponding to the actual experimental value (inset). The total current (red line) can be decomposed into intraband (green line) and interband (blue line) components, demonstrating that the kink arises from quantum interference between interband and intraband transitions. c Experimental and d theoretical 2D color map of the 7th harmonic spectra as a function of peak intensity under excitation along the zigzag direction, respectively. The color is plotted on a logarithmic scale. e Normalized 7th harmonic spectra at specific laser peak intensity corresponding to 145, 195, 210, and 255\u2009GW\/cm\u00b2, which are linecuts of (c). At low laser field strength, a single peak is observed, but as the field strength increases, this single peak begins to broaden and split into multiple peaks, indicating the emergence of an interference between different electron pathways or transitions. As the field strength further increases to 255\u2009GW\/cm\u00b2 and beyond, the formation of shoulder peaks becomes more pronounced potentially due to more complex quantum pathways or transitions. f Theoretical calculation of normalized 7th harmonic spectra at the specific laser peak intensity corresponding to 100, 375, 600 and 900\u2009GW\/cm\u00b2, which is the linecut of (d). The calculated spectra exhibit interference patterns that closely resemble the experimental observations, particularly in the peak broadening and the emergence of multiple peaks at higher field strengths. All calculations were performed using the Tight Binding model, which was employed for solving the Semiconductor Bloch Equations.<\/p>\n<p>In the perturbative regime, harmonic spectral profiles are primarily dictated by the driving pulse shape, typically exhibiting Gaussian-like profiles<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 43\" title=\"Shen, Y. R. The Principles of Nonlinear Optics. (Wiley, 2003).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#ref-CR43\" id=\"ref-link-section-d78054503e1260\" rel=\"nofollow noopener\" target=\"_blank\">43<\/a>. Beyond the perturbative regime, however, the spectral profile can also be affected by interference between multiple quantum pathways of charge carriers that emerge on sub-laser-cycle timescales. Specifically, interference between distinct quantum pathways can produce spectral fringes, including peak splitting, that reflect the complex dynamics of charge carriers (as has been observed due to other mechanisms in bulk systems<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 10\" title=\"Reisl&#xF6;hner, J., Kim, D., Babushkin, I. &amp; Pfeiffer, A. N. Onset of Bloch oscillations in the almost-strong-field regime. Nat. Commun. 13, 7716 (2022).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#ref-CR10\" id=\"ref-link-section-d78054503e1264\" rel=\"nofollow noopener\" target=\"_blank\">10<\/a>,<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" title=\"Xia, P. et al. High-harmonic generation in GaAs beyond the perturbative regime. Phys. Rev. B 104, L121202 (2021).\" href=\"#ref-CR45\" id=\"ref-link-section-d78054503e1267\">45<\/a>,<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" title=\"Sekiguchi, F. et al. Enhancing high harmonic generation in GaAs by elliptically polarized light excitation. Phys. Rev. B 108, 205201 (2023).\" href=\"#ref-CR46\" id=\"ref-link-section-d78054503e1267_1\">46<\/a>,<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 47\" title=\"Kim, Y. W. et al. Spectral interference in high harmonic generation from solids. ACS Photonics 6, 851&#x2013;857 (2019).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#ref-CR47\" id=\"ref-link-section-d78054503e1270\" rel=\"nofollow noopener\" target=\"_blank\">47<\/a>). Thus, we hypothesize that these phenomena all arise from multiple quantum path interferences. The main question is then which paths dominate the response of WS2 in this regime?<\/p>\n<p>To address this question, we perform exhaustive theoretical calculations based on several levels of theory. First, ab-initio time-dependent density functional theory (TDDFT) simulations are performed and compared with the experiment. Unfortunately, due to the very long-wavelength driving TDDFT fails to reproduce the dominant experimental features. This arises primarily because TDDFT does not include sufficient dephasing channels, which are highly relevant and can significantly alter the HHG spectra in our conditions<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 48\" title=\"Kim, Y. et al. Dephasing dynamics accessed by high harmonic generation: determination of electron&#x2013;hole decoherence of Dirac fermions. Nano Lett. 24, 1277&#x2013;1283 (2024).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#ref-CR48\" id=\"ref-link-section-d78054503e1279\" rel=\"nofollow noopener\" target=\"_blank\">48<\/a> (because a single driving field period is ~ 15\u2009fs, meaning dephasing occurs already within a single laser cycle, with recent dephasing times expected to be ~ fs on average<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 49\" title=\"Korolev, V. et al. Unveiling the Role of Electron-Phonon Scattering in Dephasing High-Order Harmonics in Solids. arXiv preprint arXiv:2401.12929 (2024).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#ref-CR49\" id=\"ref-link-section-d78054503e1283\" rel=\"nofollow noopener\" target=\"_blank\">49<\/a>). Nonetheless, the TDDFT simulations allow us to conclude that in our conditions contributions from electronic correlations and higher- or lower-order conduction and valence bands are expected to be minor in the overall response (see\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#MOESM1\" rel=\"nofollow noopener\" target=\"_blank\">SI<\/a>). Consequently, we develop a simple two-band model based on a tight-binding (TB) Hamiltonian (with an approach similar to that in refs. <a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 50\" title=\"Wang, Y. et al. Tight-binding model for electronic structure of hexagonal boron phosphide monolayer and bilayer. J. Phys.: Condens. Matter 31, 285501 (2019).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#ref-CR50\" id=\"ref-link-section-d78054503e1290\" rel=\"nofollow noopener\" target=\"_blank\">50<\/a>,<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 51\" title=\"Galler, A., Rubio, A. &amp; Neufeld, O. Mapping light-dressed floquet bands by highly nonlinear optical excitations and valley polarization. J. Phys. Chem. Lett. 14, 11298&#x2013;11304 (2023).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#ref-CR51\" id=\"ref-link-section-d78054503e1293\" rel=\"nofollow noopener\" target=\"_blank\">51<\/a> see\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#MOESM1\" rel=\"nofollow noopener\" target=\"_blank\">SI<\/a>), which we employ in semiconductor Bloch equations (SBE) in the length gauge in a density matrix formalism<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 52\" title=\"Yue, L. &amp; Gaarde, M. B. Structure gauges and laser gauges for the semiconductor Bloch equations in high-order harmonic generation in solids. Phys. Rev. A 101, 053411 (2020).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#ref-CR52\" id=\"ref-link-section-d78054503e1301\" rel=\"nofollow noopener\" target=\"_blank\">52<\/a>,<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 53\" title=\"Mrudul, M. S. &amp; Dixit, G. High-harmonic generation from monolayer and bilayer graphene. Phys. Rev. B 103, 094308 (2021).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#ref-CR53\" id=\"ref-link-section-d78054503e1304\" rel=\"nofollow noopener\" target=\"_blank\">53<\/a> (given in a.u):<\/p>\n<p>$$\\begin{array}{c}\\frac{\\partial }{\\partial {{\\rm{t}}}}{\\rho }_{{vv}}({{\\bf{k}}},t)={{\\rm{i}}}{{\\bf{E}}}(t)\\cdot \\left[{{{\\bf{d}}}}_{{{\\bf{cv}}}}\\left({{\\bf{k}}}\\right)\\,{\\rho }_{{cv}}^{*}\\left({{\\bf{k}}},t\\right)-{{{\\bf{d}}}}_{{{\\bf{cv}}}}^{*}\\,{\\rho }_{{cv}}({{\\bf{k}}},t)\\right]\\\\ \\frac{\\partial }{\\partial {{\\rm{t}}}}{\\rho }_{{{\\rm{cv}}}}\\left({{\\bf{k}}},t\\right)=\\,-{{\\rm{i}}}\\left[\\begin{array}{c}({\\varepsilon }_{{CB}}\\left({{\\bf{k}}}\\left(t\\right)\\right)-{\\varepsilon }_{{VB}}\\left({{\\bf{k}}}\\left(t\\right)\\right)-\\frac{i}{{T}_{2}}){\\rho }_{{cv}}\\left({{\\bf{k}}},t\\right)\\\\+{{\\bf{E}}}\\left({{\\rm{t}}}\\right)\\cdot \\left(\\begin{array}{c}\\left({{{\\bf{d}}}}_{{{\\bf{cc}}}}\\left({{\\bf{k}}}\\right)-{{{\\bf{d}}}}_{{{\\bf{vv}}}}\\left({{\\bf{k}}}\\right)\\right){\\rho }_{{{\\rm{cv}}}}\\left({{\\bf{k}}},{{\\rm{t}}}\\right)\\\\+{{{\\bf{d}}}}_{{{\\bf{cv}}}}\\left({{\\bf{k}}}\\right)\\left(2{\\rho }_{{{\\rm{vv}}}}\\left({{\\bf{k}}},t\\right)-1\\right)\\end{array}\\right)\\end{array}\\right]\\end{array}$$<\/p>\n<p>\n                    (1)\n                <\/p>\n<p>where \\({{\\bf{k}}}(t)={{{\\bf{k}}}}_{0}+\\frac{1}{{{\\rm{c}}}}{{\\bf{A}}}(t)\\), with \\({{{\\bf{k}}}}_{0}\\) the crystal momentum at \\(t\\,\\)=\u2009\\(0\\), and \\({{\\bf{E}}}({{\\rm{t}}})\\) the electric field vector (in the dipole approximation), which is connected to the vector potential via: \\(-{\\partial }_{{{\\rm{t}}}}{{\\bf{A}}}(t)={{\\rm{c}}}{{\\bf{E}}}(t)\\), and \\({{\\rm{c}}}\\) is the speed of light. In Eq. (<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"equation anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#Equ1\" rel=\"nofollow noopener\" target=\"_blank\">1<\/a>), \\({\\rho }_{{ij}}\\) is the density matrix, \\({\\varepsilon }_{{CB}\/{VB}}\\) is the band eigen-energy, \\({{{\\bf{d}}}}_{{{\\rm{ij}}}}\\) are transition dipole matrix elements, and \\({{{\\rm{T}}}}_{2}\\) is the phenomenological dephasing time (taken as 5\u2009fs<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 49\" title=\"Korolev, V. et al. Unveiling the Role of Electron-Phonon Scattering in Dephasing High-Order Harmonics in Solids. arXiv preprint arXiv:2401.12929 (2024).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#ref-CR49\" id=\"ref-link-section-d78054503e2316\" rel=\"nofollow noopener\" target=\"_blank\">49<\/a>). From the density matrix we obtain the time-dependent current, \\({{\\bf{J}}}\\left(t\\right)={{{\\bf{J}}}}_{{{\\bf{intra}}}}\\left(t\\right)+{{{\\bf{J}}}}_{{{\\bf{inter}}}}(t)\\) (separated to inter- intra-band contributions):<\/p>\n<p>$${{{\\bf{J}}}}_{{{\\bf{i}}}{{\\bf{n}}}{{\\bf{t}}}{{\\bf{r}}}{{\\bf{a}}}}(t) \t=-\\mathop{\\sum }\\limits_{{{\\bf{k}}}\\in {{\\rm{BZ}}}}[{\\rho }_{vv}({{\\bf{k}}},t){{{\\bf{p}}}}_{{{\\bf{v}}}{{\\bf{v}}}}({{\\bf{k}}}(t))+{\\rho }_{cc}({{\\bf{k}}},t){{{\\bf{p}}}}_{{{\\bf{c}}}{{\\bf{c}}}}({{\\bf{k}}}(t))]\\\\ {{{\\bf{J}}}}_{{{\\bf{i}}}{{\\bf{n}}}{{\\bf{t}}}{{\\bf{e}}}{{\\bf{r}}}}(t)\t=-\\mathop{\\sum }\\limits_{{{\\bf{k}}}\\in {{\\rm{BZ}}}}2{{\\rm{Re}}}[{\\rho }_{cv}({{\\bf{k}}},t){{{\\bf{p}}}}_{{{\\bf{v}}}{{\\bf{c}}}}({{\\bf{k}}}(t))]$$<\/p>\n<p>\n                    (2)\n                <\/p>\n<p>where \\({{{\\bf{p}}}}_{{{\\bf{ij}}}}\\) are the momentum matrix elements. All momentum and dipole matrix elements, as well as band energies, are obtained through analytical expressions from the TB Hamiltonian, which is optimally fitted to DFT bands throughout across entire BZ with an accurate 14th-order nearest-neighbor Hamiltonian (where spin is neglected and with the gap at K\/K\u2019 offset to match experimental values, as it is often underestimated in DFT). From \\({{\\bf{J}}}\\left(t\\right)\\) we compute the HHG spectrum as \\({{{\\rm{I}}}}_{{{\\rm{HHG}}}}\\left(\\Omega \\right)={\\left|\\int {{\\rm{dtf}}}\\left(t\\right){\\partial }_{{{\\rm{t}}}}\\,{{\\bf{J}}}\\left(t\\right){{{\\rm{e}}}}^{-{{\\rm{i}}}\\Omega {{\\rm{t}}}}\\right|}^{2}\\), with \\({{\\rm{f}}}\\left(t\\right)\\) being a super-gaussian window function. For all additional technical details of the propagation and numerical procedures see the\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#MOESM1\" rel=\"nofollow noopener\" target=\"_blank\">SI<\/a>.<\/p>\n<p>Figure\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"figure anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#Fig3\" rel=\"nofollow noopener\" target=\"_blank\">3b, d, f<\/a> present numerical results employing the SBE-TB formalism, showing strong agreement with the experiment. The simulations correctly predict the kink in the 7th harmonic yield vs. peak intensity (Fig.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"figure anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#Fig3\" rel=\"nofollow noopener\" target=\"_blank\">3d<\/a>). A pulse duration of ~ 200\u2009fs is employed to resolve the peak splitting in Fig.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"figure anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#Fig3\" rel=\"nofollow noopener\" target=\"_blank\">3d<\/a>. In the inset of Fig.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"figure anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#Fig3\" rel=\"nofollow noopener\" target=\"_blank\">3d<\/a>, we confirm that nearly the same behavior is observed for a pulse duration of ~120\u2009fs, corresponding to the actual experimental value. The total current (red line) can be decomposed into intraband (green line) and interband (blue line) components, elucidating that this effect originates from quantum interference between interband and intraband emission channels\u2014a feature absent in either channel alone and requiring their complete or partial destructive interference. This is the first observation to our knowledge of such clear interferences in 2D systems. We note that the onset intensity of this effect is overall higher in the theory, likely due to excitonic effects not captured in our simulations. Excitonic resonances can enhance carrier excitation even at lower laser intensities. Strong Coulomb interactions also give rise to tightly bound excitons in real space, which in turn promote greater momentum-space delocalization of excited photo-carriers, even without laser-field-driven intraband excitations. According to recent studies<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 54\" title=\"Mad&#xE9;o, J. et al. Directly visualizing the momentum-forbidden dark excitons and their dynamics in atomically thin semiconductors. Science 370, 1199&#x2013;1204 (2020).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#ref-CR54\" id=\"ref-link-section-d78054503e3030\" rel=\"nofollow noopener\" target=\"_blank\">54<\/a>, exciton\u2013phonon and exciton\u2013plasmon scattering processes can provide finite momentum to the carriers. Furthermore, strong-laser-field-driven exciton ionization processes<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 36\" title=\"Kobayashi, Y. et al. Floquet engineering of strongly driven excitons in monolayer tungsten disulfide. Nat. Phys. &#010;                  https:\/\/doi.org\/10.1038\/s41567-022-01849-9&#010;                  &#010;                 (2023).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#ref-CR36\" id=\"ref-link-section-d78054503e3035\" rel=\"nofollow noopener\" target=\"_blank\">36<\/a> can open additional HHG pathways that are not captured by the current theory. To accurately address the issues above, time-resolved photoemission spectroscopy or time-resolved absorption spectroscopy under identical mid-infrared excitation can provide direct access to the probe excitonic states and carrier scattering dynamics in the time domain. However, such an investigation goes beyond the scope of the present study.<\/p>\n<p>Theoretical analysis of HHG in monolayer WS2<\/p>\n<p>At the next stage, our theory reproduces the peak broadening and splitting dynamics vs. laser intensity (see Fig.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"figure anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#Fig3\" rel=\"nofollow noopener\" target=\"_blank\">3a\u2013d<\/a>)). Note that here we employed much longer driving laser pulses in order to obtain sufficient spectral resolution (~200\u2009fs FWHM), but otherwise employed the same conditions as in the experiment. In the simulations, such long timescale dynamics are necessary to be able to resolve peak splitting on an energy scale of ~0.02\u2009eV. Our theoretical analysis reveals that the splitting and converging dynamics do not arise solely due to interference of interband and intraband channels, as the effect appears in each channel separately (see\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"supplementary material anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#MOESM1\" rel=\"nofollow noopener\" target=\"_blank\">SI<\/a> for 7th harmonic spectrum from interband and intraband channels). To gain further insight, we perform a comprehensive k-resolved analysis of the HHG yield, and uncover that at the onset of the peak splitting, a substantial portion of the BZ is excited (comparing occupations in Fig.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"figure anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#Fig4\" rel=\"nofollow noopener\" target=\"_blank\">4a, b<\/a>, middle panel). Indeed, at high laser powers, electrons occupy not only regions near K\/K\u2019 valleys, but also towards \\(\\Gamma\\) and M points. The HHG emission from these regions is comparable to that from the K\/K\u2032 valleys and, under certain conditions, can be even stronger. Mathematically, this is clear due to the relatively low optical gap throughout the BZ (e.g., the gap at \\(\\Gamma\\) is\u2009~\u20093\u2009eV, only ~1\u2009eV higher than the gap at K\/K\u2019). The detailed spectral profiles are determined by the magnitudes and phases of the HHG emission, which depend on specific laser excitation conditions including finite beam size, temporal and spectral pulse profiles<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 45\" title=\"Xia, P. et al. High-harmonic generation in GaAs beyond the perturbative regime. Phys. Rev. B 104, L121202 (2021).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#ref-CR45\" id=\"ref-link-section-d78054503e3096\" rel=\"nofollow noopener\" target=\"_blank\">45<\/a>,<a data-track=\"click\" data-track-action=\"reference anchor\" data-track-label=\"link\" data-test=\"citation-ref\" aria-label=\"Reference 55\" title=\"Floss, I. et al. Ab initio multiscale simulation of high-order harmonic generation in solids. Phys. Rev. A 97, 011401 (2018).\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#ref-CR55\" id=\"ref-link-section-d78054503e3099\" rel=\"nofollow noopener\" target=\"_blank\">55<\/a>. Nevertheless, this result clearly indicates that the peak splitting originates from quantum interference of laser-field-driven carriers occupying multiple k-points including regions near \\(\\Gamma\\) and M points.<\/p>\n<p>Fig. 4: Theory of peak splitting in HHG from WS2.<a class=\"c-article-section__figure-link\" data-test=\"img-link\" data-track=\"click\" data-track-label=\"image\" data-track-action=\"view figure\" href=\"https:\/\/www.nature.com\/articles\/s41467-025-65725-9\/figures\/4\" rel=\"nofollow noopener\" target=\"_blank\"><img decoding=\"async\" aria-describedby=\"Fig4\" src=\"https:\/\/www.newsbeep.com\/uk\/wp-content\/uploads\/2025\/11\/41467_2025_65725_Fig4_HTML.png\" alt=\"figure 4\" loading=\"lazy\" width=\"685\" height=\"535\"\/><\/a><\/p>\n<p>a SBE simulated 7th harmonic spectrum (left), showing no onset of peak splitting at lower power (100\u2009GW\/cm2). Middle panel shows the k-resolved contributions to this peak, indicating mostly localized charge carrier excitation and emission from the K\/K\u2019 valleys. Right panel shows the optical gap throughout the BZ in this system. The color is plotted on a linear scale for both middle and right panel. b Same as (a) for higher driving power (375\u2009GW\/cm2) where there is peak-splitting occurring. Here, emission is contributed form delocalized regions in the BZ, including from \u0393 and M. The evenly spaced interference pattern in k-space presumably indicates regions with constructive\/destructive interference due to the phase of the harmonic emission. c Same as (b) but with the modified TB model (see text) that reproduced the electronic structure in WS2 only near the K\/K\u2019 valleys (see right panel), where peak splitting does not occur. The white hexagon shows the outline of the first Brillouin zone edge.<\/p>\n<p>This conclusion is further validated by performing additional simulations where the TB Hamiltonian is modified to reproduce the correct electronic structure only near K\/K\u2019 valleys, while the gap is artificially increased towards \\(\\Gamma\\) and M to suppress their contribution (see right panels in Fig.\u00a0<a data-track=\"click\" data-track-label=\"link\" data-track-action=\"figure anchor\" href=\"http:\/\/www.nature.com\/articles\/s41467-025-65725-9#Fig4\" rel=\"nofollow noopener\" target=\"_blank\">4b, c<\/a>). Indeed, in these conditions, the peak splitting phenomena are completely suppressed at identical laser power, corroborating that interference of emission between different points in the BZ accounts for the physical mechanism of peak splitting (and that specifically the K\/K\u2019 valleys, including their Berry curvature, cannot alone account for the effect). The peak closing dynamics at yet higher driving is seen to arise due to increased dominance of the intraband emission channel where the split peak converges.<\/p>\n","protected":false},"excerpt":{"rendered":"Transition from perturbative to strong-field driven HHG in monolayer WS2 Figure\u00a01a schematically illustrates the electronic processes in monolayer&hellip;\n","protected":false},"author":2,"featured_media":250372,"comment_status":"","ping_status":"","sticky":false,"template":"","format":"standard","meta":{"footnotes":""},"categories":[24],"tags":[38911,4230,4231,2302,90,24549,56,54,55],"class_list":{"0":"post-250371","1":"post","2":"type-post","3":"status-publish","4":"format-standard","5":"has-post-thumbnail","7":"category-physics","8":"tag-high-harmonic-generation","9":"tag-humanities-and-social-sciences","10":"tag-multidisciplinary","11":"tag-physics","12":"tag-science","13":"tag-two-dimensional-materials","14":"tag-uk","15":"tag-united-kingdom","16":"tag-unitedkingdom"},"_links":{"self":[{"href":"https:\/\/www.newsbeep.com\/uk\/wp-json\/wp\/v2\/posts\/250371","targetHints":{"allow":["GET"]}}],"collection":[{"href":"https:\/\/www.newsbeep.com\/uk\/wp-json\/wp\/v2\/posts"}],"about":[{"href":"https:\/\/www.newsbeep.com\/uk\/wp-json\/wp\/v2\/types\/post"}],"author":[{"embeddable":true,"href":"https:\/\/www.newsbeep.com\/uk\/wp-json\/wp\/v2\/users\/2"}],"replies":[{"embeddable":true,"href":"https:\/\/www.newsbeep.com\/uk\/wp-json\/wp\/v2\/comments?post=250371"}],"version-history":[{"count":0,"href":"https:\/\/www.newsbeep.com\/uk\/wp-json\/wp\/v2\/posts\/250371\/revisions"}],"wp:featuredmedia":[{"embeddable":true,"href":"https:\/\/www.newsbeep.com\/uk\/wp-json\/wp\/v2\/media\/250372"}],"wp:attachment":[{"href":"https:\/\/www.newsbeep.com\/uk\/wp-json\/wp\/v2\/media?parent=250371"}],"wp:term":[{"taxonomy":"category","embeddable":true,"href":"https:\/\/www.newsbeep.com\/uk\/wp-json\/wp\/v2\/categories?post=250371"},{"taxonomy":"post_tag","embeddable":true,"href":"https:\/\/www.newsbeep.com\/uk\/wp-json\/wp\/v2\/tags?post=250371"}],"curies":[{"name":"wp","href":"https:\/\/api.w.org\/{rel}","templated":true}]}}