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Main Authors: Duncan, C. J. R., Johnson, A. C., Maity, I., Rubio, A., Gordon, M., Bartnik, A. C., Kaemingk, M., Li, W. H., Andorf, M. B., Pennington, C. A., Bazarov, I. V., Tate, M. W., Muller, D. A., Thom-Levy, J., Gruner, S. M., Lindenberg, A . M., Liu, F., Maxson, J. M.
Format: Preprint
Published: 2025
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Online Access:https://arxiv.org/abs/2502.11452
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author Duncan, C. J. R.
Johnson, A. C.
Maity, I.
Rubio, A.
Gordon, M.
Bartnik, A. C.
Kaemingk, M.
Li, W. H.
Andorf, M. B.
Pennington, C. A.
Bazarov, I. V.
Tate, M. W.
Muller, D. A.
Thom-Levy, J.
Gruner, S. M.
Lindenberg, A . M.
Liu, F.
Maxson, J. M.
author_facet Duncan, C. J. R.
Johnson, A. C.
Maity, I.
Rubio, A.
Gordon, M.
Bartnik, A. C.
Kaemingk, M.
Li, W. H.
Andorf, M. B.
Pennington, C. A.
Bazarov, I. V.
Tate, M. W.
Muller, D. A.
Thom-Levy, J.
Gruner, S. M.
Lindenberg, A . M.
Liu, F.
Maxson, J. M.
contents Two-dimensional moiré materials are formed by artificially stacking atomically thin monolayers. A wealth of correlated and topological quantum phases can be engineered via precise choice of stacking geometry. These designer electronic properties depend crucially on interlayer coupling and atomic registry. An important open question is how atomic registry responds on ultrafast timescales to optical excitation and whether the moiré geometry can be dynamically reconfigured to tune emergent phenomena in real time. Here we show that femtosecond photoexcitation drives a coherent twist-untwist motion of the moiré superlattice in $2^\circ$ and $57^\circ$ twisted WSe$_2$/MoSe$_2$ heterobilayers, resolved directly by ultrafast electron diffraction. Upon above-band-gap photoexcitation, the moiré superlattice diffraction features are enhanced within 1 ps and subsequently suppressed several picoseconds after, deviating markedly from typical photoinduced lattice heating. Kinetic diffraction analysis, supported by simulations of the sample dynamics, indicates a peak-to-trough local twist angle modulation of $0.6^\circ$, correlated with a sub-THz frequency moiré phonon. This motion is driven by ultrafast charge transfer that transiently increases interlayer attraction. Our results could lead to ultrafast control of moiré periodic lattice distortions and, by extension, the local moiré potential that shapes excitons, polarons, and correlation-driven behaviors
format Preprint
id arxiv_https___arxiv_org_abs_2502_11452
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Photoinduced twist and untwist of moiré superlattices in TMDC heterobilayers
Duncan, C. J. R.
Johnson, A. C.
Maity, I.
Rubio, A.
Gordon, M.
Bartnik, A. C.
Kaemingk, M.
Li, W. H.
Andorf, M. B.
Pennington, C. A.
Bazarov, I. V.
Tate, M. W.
Muller, D. A.
Thom-Levy, J.
Gruner, S. M.
Lindenberg, A . M.
Liu, F.
Maxson, J. M.
Materials Science
Two-dimensional moiré materials are formed by artificially stacking atomically thin monolayers. A wealth of correlated and topological quantum phases can be engineered via precise choice of stacking geometry. These designer electronic properties depend crucially on interlayer coupling and atomic registry. An important open question is how atomic registry responds on ultrafast timescales to optical excitation and whether the moiré geometry can be dynamically reconfigured to tune emergent phenomena in real time. Here we show that femtosecond photoexcitation drives a coherent twist-untwist motion of the moiré superlattice in $2^\circ$ and $57^\circ$ twisted WSe$_2$/MoSe$_2$ heterobilayers, resolved directly by ultrafast electron diffraction. Upon above-band-gap photoexcitation, the moiré superlattice diffraction features are enhanced within 1 ps and subsequently suppressed several picoseconds after, deviating markedly from typical photoinduced lattice heating. Kinetic diffraction analysis, supported by simulations of the sample dynamics, indicates a peak-to-trough local twist angle modulation of $0.6^\circ$, correlated with a sub-THz frequency moiré phonon. This motion is driven by ultrafast charge transfer that transiently increases interlayer attraction. Our results could lead to ultrafast control of moiré periodic lattice distortions and, by extension, the local moiré potential that shapes excitons, polarons, and correlation-driven behaviors
title Photoinduced twist and untwist of moiré superlattices in TMDC heterobilayers
topic Materials Science
url https://arxiv.org/abs/2502.11452