Shaping exciton polarization dynamics in 2D semiconductors by tailored ultrafast pulses

Omri Meron; Uri Arieli; Eyal Bahar; Swarup Deb; Moshe Ben Shalom; Haim Suchowski

doi:10.1038/s41377-025-01748-7

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Shaping exciton polarization dynamics in 2D semiconductors by tailored ultrafast pulses

Original Articles

- Shaping exciton polarization dynamics in 2D semiconductors by tailored ultrafast pulses
- Shaping exciton polarization dynamics in 2D semiconductors by tailored ultrafast pulses
- LSA 2025年14卷第3期页码：831-838
- Affiliations：
  
  1.School of Physics and Astronomy, Faculty of Exact Sciences, Tel Aviv University, Tel‐Aviv 6997801, Israel
  2.Center for Light‐Matter Interaction, Tel Aviv University, Tel‐Aviv 6997801, Israel
- Author bio：
  
  Omri Meron (omrimeron@tauex.tau.ac.il)
- Funds：
- DOI：10.1038/s41377-025-01748-7
  中图分类号：
- 收稿日期：2024-08-29，
  
  修回日期：2024-11-14，
  
  录用日期：2025-01-06，
  
  网络出版日期：2025-02-11，
  
  纸质出版日期：2025-03-31
- Accepted：
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Shaping exciton polarization dynamics in 2D semiconductors by tailored ultrafast pulses[J]. LSA, 2025,14(3):831-838.

Meron, O. et al. Shaping exciton polarization dynamics in 2D semiconductors by tailored ultrafast pulses. Light: Science & Applications, 14, 831-838 (2025).
Shaping exciton polarization dynamics in 2D semiconductors by tailored ultrafast pulses[J]. LSA, 2025,14(3):831-838. DOI： 10.1038/s41377-025-01748-7.

Meron, O. et al. Shaping exciton polarization dynamics in 2D semiconductors by tailored ultrafast pulses. Light: Science & Applications, 14, 831-838 (2025). DOI： 10.1038/s41377-025-01748-7.

摘要

Abstract

The ultrafast formation of strongly bound excitons in two-dimensional semiconductors provides a rich platform for studying fundamental physics as well as developing novel optoelectronic technologies. While extensive research has explored the excitonic coherence

many-body interactions

and nonlinear optical properties

the potential to study these phenomena by directly controlling their coherent polarization dynamics has not been fully realized. In this work

we use a sub-10 fs pulse shaper to study how temporal control of coherent exciton polarization affects the generation of four-wave mixing in monolayer WSe

under ambient conditions. By tailoring multiphoton pathway interference

we tune the nonlinear response from d

estructive to constructive interference

resulting in a 2.6-fold enhancement over the four-wave mixing generated by a transform-limited pulse. This demonstrates a general method for nonlinear enhancement by shaping the pulse to counteract the temporal dispersion experienced during resonant light–matter interactions. Our method allows us to excite both 1s and 2s states

showcasing a selective control over the resonant state that produces nonlinearity. By comparing our results with theory

we find that exciton-exciton interactions dominate the nonlinear response

rather than Pauli blocking. This capability to manipulate exciton polarization dynamics in atomically thin crystals lays the groundwork for exploring a wide range of resonant phenomena in condensed matter systems and opens up new possibilities for precise optical control in advanced optoelectronic devices.

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references

Goswami, D. Optical pulse shaping approaches to coherent control. Phys. Rep. 374 , 385–481 (2003)..

Silberberg, Y. Quantum coherent control for nonlinear spectroscopy and microscopy. Annu. Rev. Phys. Chem. 60 , 277–292 (2009)..

Brash, A. J., Liu, F. & Fox, A. M. Ultrafast manipulation of excitons and spins in quantum dots. in Quantum Dots for Quantum Information Technologies (ed Michler, P.) (Springer, Cham, 2017) pp 325–357.

Dudovich, N., Oron, D. & Silberberg, Y. Coherent transient enhancement of optically induced resonant transitions. Phys. Rev. Lett. 88 , 123004 (2002)..

Dudovich, N., Oron, D. & Silberberg, Y. Single-pulse coherently controlled nonlinear Raman spectroscopy and microscopy. Nature 418 , 512–514 (2002)..

Chelkowski, S., Bandrauk, A. D. & Corkum, P. B. Efficient molecular dissociation by a chirped ultrasho rt infrared laser pulse. Phys. Rev. Lett. 65 , 2355–2358 (1990)..

Assion, A. et al. Control of chemical reactions by feedback-optimized phase-shaped femtosecond laser pulses. Science 282 , 919–922 (1998)..

Levin, L. et al. Coherent control of bond making. Phys. Rev. Lett. 114 , 233003 (2015)..

Chernikov, A. et al. Exciton binding energy and nonhydrogenic Rydberg series in monolayer WS 2 . Phys. Rev. Lett. 113 , 076802 (2014)..

Mueller, T. & Malic, E. Exciton physics and device application of two-dimensional transition metal dichalcogenide semiconductors. npj 2D Mater. Appl. 2 , 29 (2018)..

Brem, S. et al. Intrinsic lifetime of higher excitonic states in tungsten diselenide monolayers. Nanoscale 11 , 12381–12387 (2019)..

Mak, K. F. et al. Atomically thin MoS 2 : a new direct-gap semiconductor. Phys. Rev. Lett. 105 , 136805 (20 10)..

Amani, M. et al. Near-unity photoluminescence quantum yield in MoS 2 . Science 350 , 1065–1068 (2015)..

Geim, A. K. & Grigorieva, I. V. Van der Waals heterostructures. Nature 499 , 419–425 (2013)..

Ciarrocchi, A. et al. Excitonic devices with Van der Waals heterostructures: valleytronics meets twistronics. Nat. Rev. Mater. 7 , 449–464 (2022)..

Chaves, A. et al. Bandgap engineering of two-dimensional semiconductor materials. npj 2D Mater. Appl. 4 , 29 (2020)..

Moody, G. et al. Intrinsic homogeneous linewidth and broadening mechanisms of excitons in monolayer transition metal dichalcogenides. Nat. Commun. 6 , 8315 (2015)..

Poellmann, C. et al. Resonant internal quantum transitions and femtosecond radiative decay of excitons in monolayer WSe 2 . Nat. Mater. 14 , 889–893 (2015)..

Dey, P. et al. Optical coherence in atomic-monolayer transition-metal dichalcogenides limited by electron-phonon interactions. Phys. Rev. Lett. 116 , 127402 (2016)..

Jakubczyk, T. et al. Radiatively limited dephasing and exciton dynamics in MoSe 2 monolayers revealed with four-wave mixing microscopy. Nano Lett. 16 , 5333–5339 (2016)..

Steinleitner, P. et al. Direct observation of ultrafast exciton formation in a monolayer of WSe 2 . Nano Lett. 17 , 1455–1460 (2017)..

Trovatello, C. et al. The ultrafast onset of exciton formation in 2D semiconductors. Nat. Commun. 11 , 5277 (2020)..

Li, D. H. et al. Exciton–phonon coupling strength in single-layer MoSe 2 at room temperature. Nat. Commun. 12 , 954 (2021)..

Bauer, J. M. et al. Excitonic resonances control the temporal dynamics of nonlinear optical wave mixing in monolayer semiconductors. Nat. Photonics 16 , 777–783 (2022)..

Purz, T. L. et al. Imaging dynamic exciton interactions and coupling in transition metal dichalcogenides. J. Chem. Phys. 156 , 214704 (2022)..

Luo, W. J. et al. Ultrafast nanoimaging of electronic coherence of monolayer WSe 2 . Nano Lett. 23 , 1767–1773 (2023)..

Rodek, A. et al. Controlled coherent-coupling and dynamics of exciton complexes in a MoSe 2 monolayer. 2D Mater. 10 , 025027 (2023)..

Dudovich, N. et al. Transform-limited pulses are not optimal for resonant multiphoton transitions. Phys. Rev. Lett. 86 , 47–50 (2001)..

Bahar, E. et al. Unlocking coherent control of ultrafast plasmonic interaction. Laser Photonics Rev. 16 , 2100467 (2022)..

Dai, Y. Y. et al. Broadband plasmon-enhanced four-wave mixing in monolayer MoS 2 . Nano Lett. 21 , 6321–6327 (2021)..

Malard, L. M. et al. Studying 2D materials with advanced Raman spectroscopy: CARS, SRS and TERS. Phys. Chem. Chem. Phys. 23 , 23428–23444 (2021)..

Liu, H. Z. et al. High-harmonic generation from an atomically thin semiconductor. Nat. Phys. 13 , 262–265 (2017)..

Trovatello, C. et al. Optical parametric amplification by monolayer transition metal dichalcogenides. Nat. Photonics 15 , 6–10 (2021)..

Weiner, A. M. Femtosecond pulse shaping using spatial light modulators. Rev. Sci. Instrum. 71 , 1929–1960 (2000)..

Gu, H. G. et al. Layer-dependent dielectric and optical properties of centimeter-scale 2D WSe 2 : evolution from a single layer to few layers. Nanoscale 11 , 22762–22771 (2019)..

Suchowski, H. et al. Phase mismatch–free nonlinear propagation in optical zero-index materials. Science 342 , 1223–1226 (2013)..

Kravtsov, V. et al. Plasmonic nanofocused four-wave mixing for femtosecond near-field imaging. Nat. Nanotechnol. 11 , 459–464 (2016)..

Katsch, F., Selig, M. & Knorr, A. Theory of coherent pump-probe spectroscopy in monolayer transition metal dichalcogenides. 2D Mater. 7 , 015021 (2019)..

Katsch, F., Selig, M. & Knorr, A. Exciton-scattering-induced dephasing in two-dimensional semiconductors. Phys. Rev. Lett. 124 , 257402 (2020)..

Madéo, J. et al. Directly visualizing the momentum-forbidden dark excitons and their dynamics in atomically thin semiconductors. Science 370 , 1199–1204 (2020)..

Riche, F. et al. Robust room temperature emissions of trion in darkish WSe 2 monolayers: effects of dark neutral and charged excitonic states. J. Phys. 32 , 365702 (2020)..

Yao, K. Y. et al. Continuous Wave sum frequency generation and imaging of monolayer and heterobilayer two-dimensional semiconductors. ACS Nano 14 , 708–714 (2020)..

Lin, K. Q. et al. Narrow-band high-lying excitons with negative-mass electrons in monolayer WSe 2 . Nat. Commun. 12 , 5500 (2021)..

Hao, K. et al. Neutral and charged inter-valley biexcitons in monolayer MoSe 2 . Nat. Commun. 8 , 15552 (2017)..

Oron, D., Dudovich, N. & Silberberg, Y. Single-pulse phase-contrast nonlinear Raman spectroscopy. Phys. Rev. Lett. 89 , 273001 (2002)..

Wang, C. F. & El-Khoury, P. Z. Resonant coherent Raman scattering from WSe 2 . J. Phys. Chem. A 126 , 5832–5836 (2022)..

He, K. L. et al. Tightly bound excitons in monolayer WSe 2 . Phys. Rev. Lett. 113 , 026803 (2014)..

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