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  • Letter
  • Open Access

Ultrafast charge transfer dynamics at the MoS2/Au interface observed via optical spectroscopy under ambient conditions

Tao Yang1,*, Zhipeng Huang1, Stephan Sleziona1, Eckart Hasselbrink2, Peter Kratzer1, Marika Schleberger1, R. Kramer Campen1, and Yujin Tong1,†

  • *Contact author: tao.yang@uni-due.de
  • †Contact author: yujin.tong@uni-due.de

Phys. Rev. B 114, L051406 – Published 27 July, 2026

DOI: https://doi.org/10.1103/t3fz-gqf9

Abstract

Integrating atomically thin transition metal dichalcogenides (TMDCs) with metallic surfaces is an effective strategy to leverage their exceptional properties in advanced devices and catalysts, as it promotes efficient charge carrier injection and extraction from TMDC monolayers. Light-matter interactions in TMDC monolayers predominantly occur at the K point, making the charge carrier dynamics at this point essential for optimizing charge transfer efficiency. However, direct probing of the dynamics at the K point of TMDCs interfaced with metal substrates remains challenging. In this Letter, we employed pump-probe azimuth- and polarization-dependent final-state sum frequency generation spectroscopy to investigate the ultrafast dynamics of charge transfer at the K point of a MoS2 monolayer on an Au substrate. We observed ultrafast injection of photoexcited hot electrons from Au into the monolayer MoS2 conduction band minimum, followed by a fast return (∼2 ps) and a trap-state-mediated slow return (∼60 ps) processes, driven by an internal electric field. The direct optical observation of the full electron dynamics at the K point of MoS2 monolayer in ambient conditions provides valuable insights into optimizing the transfer of charge carrier across the TMDC/metal interface through optimized contacts, informing the design of advanced TMDC-based devices with enhanced charge transfer rates.

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References (53)

  1. Q. H. Wang, K. Kalantar-Zadeh, A. Kis, J. N. Coleman, and M. S. Strano, Electronics and optoelectronics of two-dimensional transition metal dichalcogenides, Nat. Nanotechnol. 7, 699 (2012).
  2. T. Mueller and E. Malic, Exciton physics and device application of two-dimensional transition metal dichalcogenide semiconductors, npj 2D Mater Appl 2, 29 (2018).
  3. D. B. Sulas-Kern, E. M. Miller, and J. L. Blackburn, Photoinduced charge transfer in transition metal dichalcogenide heterojunctions–towards next generation energy technologies, Energy Environ. Sci. 13, 2684 (2020).
  4. X. Guo, Q. Li, Y. Liu, T. Jin, Y. Chen, L. Guo, and T. Lian, Enhanced light-driven charge separation and H2 generation efficiency in WSe2 nanosheet–semiconductor nanocrystal heterostructures, ACS Appl. Mater. Interfaces 12, 44769 (2020).
  5. D. K. Schroder, Semiconductor Material and Device Characterization (Wiley, Hoboken, NJ, 2006).
  6. W. Li, Y. Liang, D. Yu, L. Peng, K. P. Pernstich, T. Shen, A. R. Hight Walker, G. Cheng, C. A. Hacker, C. A. Richter, Q. Li, D. J. Gundlach, and X. Liang, Ultraviolet/ozone treatment to reduce metal-graphene contact resistance, Appl. Phys. Lett. 102, 183110 (2013).
  7. M. Chhowalla, D. Jena, and H. Zhang, Two-dimensional semiconductors for transistors, Nat. Rev. Mater. 1, 16052 (2016).
  8. Y. Wang, J. C. Kim, R. J. Wu, J. Martinez, X. Song, J. Yang, F. Zhao, A. Mkhoyan, H. Y. Jeong, and M. Chhowalla, Van der Waals contacts between three-dimensional metals and two-dimensional semiconductors, Nature (London) 568, 70 (2019).
  9. P.-C. Shen, C. Su, Y. Lin, A.-S. Chou, C.-C. Cheng, J.-H. Park, M.-H. Chiu, A.-Y. Lu, H.-L. Tang, M. M. Tavakoli, G. Pitner, X. Ji, Z. Cai, N. Mao, J. Wang, V. Tung, J. Li, J. Bokor, A. Zettl, C.-I. Wu, T. Palacios, L.-J. Li, and J. Kong, Ultralow contact resistance between semimetal and monolayer semiconductors, Nature (London) 593, 211 (2021).
  10. C. Xu, H. W. Yong, J. He, R. Long, A. R. Cadore, I. Paradisanos, A. K. Ott, G. Soavi, S. Tongay, G. Cerullo, A. C. Ferrari, O. V. Prezhdo, and Z.-H. Loh, Weak distance dependence of hot-electron-transfer rates at the interface between monolayer MoS2 and gold, ACS Nano 15, 819 (2021).
  11. R. T. Tung, The physics and chemistry of the Schottky barrier height, Appl. Phys. Rev. 1, 011304 (2014).
  12. A. Pelella, O. Kharsah, A. Grillo, F. Urban, M. Passacantando, F. Giubileo, L. Iemmo, S. Sleziona, E. Pollmann, L. Madauß, M. Schleberger, and A. Di Bartolomeo, Electron irradiation of metal contacts in monolayer MoS2 field-effect transistors, ACS Appl. Mater. Interfaces 12, 40532 (2020).
  13. F. Ceballos, Q. Cui, M. Z. Bellus, and H. Zhao, Exciton formation in monolayer transition metal dichalcogenides, Nanoscale 8, 11681 (2016).
  14. P. Steinleitner, P. Merkl, P. Nagler, J. Mornhinweg, C. Schüller, T. Korn, A. Chernikov, and R. Huber, Direct observation of ultrafast exciton formation in a monolayer of WSe2, Nano Lett. 17, 1455 (2017).
  15. G. Wang, A. Chernikov, M. M. Glazov, T. F. Heinz, X. Marie, T. Amand, and B. Urbaszek, Colloquium: Excitons in atomically thin transition metal dichalcogenides, Rev. Mod. Phys. 90, 021001 (2018).
  16. J. Madéo, M. K. L. Man, C. Sahoo, M. Campbell, V. Pareek, E. L. Wong, A. Al-Mahboob, N. S. Chan, A. Karmakar, B. M. K. Mariserla, X. Li, T. F. Heinz, T. Cao, and K. M. Dani, Directly visualizing the momentum-forbidden dark excitons and their dynamics in atomically thin semiconductors, Science 370, 1199 (2020).
  17. C. Trovatello, F. Katsch, N. J. Borys, M. Selig, K. Yao, R. Borrego-Varillas, F. Scotognella, I. Kriegel, A. Yan, A. Zettl, P. J. Schuck, A. Knorr, G. Cerullo, and S. D. Conte, The ultrafast onset of exciton formation in 2D semiconductors, Nat. Commun. 11, 5277 (2020).
  18. S. Dong, M. Puppin, T. Pincelli, S. Beaulieu, D. Christiansen, H. Hübener, C. W. Nicholson, R. P. Xian, M. Dendzik, Y. Deng, Y. W. Windsor, M. Selig, E. Malic, A. Rubio, A. Knorr, M. Wolf, L. Rettig, and R. Ernstorfer, Direct measurement of key exciton properties: Energy, dynamics, and spatial distribution of the wave function, Nat. Sci. 1, e10010 (2021).
  19. J. E. Zimmermann, M. Axt, F. Mooshammer, P. Nagler, C. Schüller, T. Korn, U. Höfer, and G. Mette, Ultrafast charge-transfer dynamics in twisted MoS2/WSe2 heterostructures, ACS Nano 15, 14725 (2021).
  20. R. Wallauer, R. Perea-Causin, L. Münster, S. Zajusch, S. Brem, J. Güdde, K. Tanimura, K.-Q. Lin, R. Huber, E. Malic, and U. Höfer, Momentum-resolved observation of exciton formation dynamics in monolayer WS2, Nano Lett. 21, 5867 (2021).
  21. A. Singh, G. Moody, K. Tran, M. E. Scott, V. Overbeck, G. Berghäuser, J. Schaibley, E. J. Seifert, D. Pleskot, N. M. Gabor, J. Yan, D. G. Mandrus, M. Richter, E. Malic, X. Xu, and X. Li, Trion formation dynamics in monolayer transition metal dichalcogenides, Phys. Rev. B 93, 041401(R) (2016).
  22. Y. Yu, Z. Ji, S. Zu, B. Du, Y. Kang, Z. Li, Z. Zhou, K. Shi, and Z. Fang, Ultrafast plasmonic hot electron transfer in Au nanoantenna/MoS2 heterostructures, Adv. Funct. Mater. 26, 6394 (2016).
  23. X. Wen, S. Chen, J. Zhao, W. Du, and W. Zhao, Enhanced plasmonic hot-carrier transfer in Au/WS2 heterojunctions under nonequilibrium condition, ACS Photonics 9, 1522 (2022).
  24. T. Pincelli, T. Vasileiadis, S. Dong, S. Beaulieu, M. Dendzik, D. Zahn, S.-E. Lee, H. Seiler, Y. Qi, R. P. Xian, J. Maklar, E. Coy, N. S. Mueller, Y. Okamura, S. Reich, M. Wolf, L. Rettig, and R. Ernstorfer, Observation of multi-directional energy transfer in a hybrid plasmonic–excitonic nanostructure, Adv. Mater. 35, 2209100 (2023).
  25. A. G. Čabo, J. A. Miwa, S. S. Grønborg, J. M. Riley, J. C. Johannsen, C. Cacho, O. Alexander, R. T. Chapman, E. Springate, M. Grioni, J. V. Lauritsen, P. D. C. King, P. Hofmann, and S. Ulstrup, Observation of ultrafast free carrier dynamics in single layer MoS2, Nano Lett. 15, 5883 (2015).
  26. F. Liu, Time- and angle-resolved photoemission spectroscopy (TR-ARPES) of TMDC monolayers and bilayers, Chem. Sci. 14, 736 (2023).
  27. K. F. Mak and J. Shan, Photonics and optoelectronics of 2D semiconductor transition metal dichalcogenides, Nat. Photon. 10, 216 (2016).
  28. D. Xiao, G.-B. Liu, W. Feng, X. Xu, and W. Yao, Coupled spin and valley physics in monolayers of MoS2 and other Group-VI dichalcogenides, Phys. Rev. Lett. 108, 196802 (2012).
  29. T. Handa, M. Holbrook, N. Olsen, L. N. Holtzman, L. Huber, H. I. Wang, M. Bonn, K. Barmak, J. C. Hone, A. N. Pasupathy, and X. Zhu, Spontaneous exciton dissociation in transition metal dichalcogenide monolayers, Sci. Adv. 10, eadj4060 (2024).
  30. T. Yang, E. Pollmann, S. Sleziona, E. Hasselbrink, P. Kratzer, M. Schleberger, R. K. Campen, and Y. Tong, Interaction between a gold substrate and monolayer MoS2: An azimuthal-dependent sum frequency generation study, Phys. Rev. B 107, 155433 (2023).
  31. T. Yang, S. Sleziona, E. Pollmann, E. Hasselbrink, P. Kratzer, M. Schleberger, R. K. Campen, and Y. Tong, Isolating the optical response of a MoS2 monolayer under extreme screening of a metal substrate, Phys. Rev. B 109, L161402 (2024).
  32. C. Hong, H. Kim, Y. Tao, J. H. Lim, J. Y. Lee, and J.-H. Kim, Ultrafast hot carrier extraction and diffusion at the MoS2/Au van der Waals electrode interface, Sci. Adv. 11, eadr1534 (2025).
  33. See Supplemental Material at http://link.aps.org/supplemental/10.1103/t3fz-gqf9 for experimental and theoretical information, which includes details about sample preparation and characterization, laser setup, data analysis, and determination of the σ of the Gaussian function for fitting. Furthermore, a simple kinetic model was applied to understand the charge transfer between Au and MoS2, which also contains Ref. [53].
  34. N. Kumar, S. Najmaei, Q. Cui, F. Ceballos, P. M. Ajayan, J. Lou, and H. Zhao, Second harmonic microscopy of monolayer MoS2, Phys. Rev. B 87, 161403(R) (2013).
  35. Y. Li, Y. Rao, K. F. Mak, Y. You, S. Wang, C. R. Dean, and T. F. Heinz, Probing symmetry properties of few-layer MoS2 and h-BN by optical second-harmonic generation, Nano Lett. 13, 3329 (2013).
  36. L. M. Malard, T. V. Alencar, A. P. M. Barboza, K. F. Mak, and A. M. de Paula, Observation of intense second harmonic generation from MoS2 atomic crystals, Phys. Rev. B 87, 201401(R) (2013).
  37. Z. Wang, C. Hong, Z. Sun, S. Wu, B. Liang, X. Duan, W.-T. Liu, and S. Wu, Contrast-enhanced phase-resolved second harmonic generation microscopy, Opt. Lett. 49, 2117 (2024).
  38. W. S. Fann, R. Storz, H. W. K. Tom, and J. Bokor, Electron thermalization in gold, Phys. Rev. B 46, 13592 (1992).
  39. J. Hohlfeld, S. S. Wellershoff, J. Güdde, U. Conrad, V. Jähnke, and E. Matthias, Electron and lattice dynamics following optical excitation of metals, Chem. Phys. 251, 237 (2000).
  40. M. Bauer, A. Marienfeld, and M. Aeschlimann, Hot electron lifetimes in metals probed by time-resolved two-photon photoemission, Prog. Surf. Sci. 90, 319 (2015).
  41. B. Liu, W. Zhao, Z. Ding, I. Verzhbitskiy, L. Li, J. Lu, J. Chen, G. Eda, and K. P. Loh, Engineering bandgaps of monolayer MoS2 and WS2 on fluoropolymer substrates by electrostatically tuned many-body effects, Adv. Mater. 28, 6457 (2016).
  42. P. Majchrzak, K. Volckaert, A. G. Čabo, D. Biswas, M. Bianchi, S. K. Mahatha, M. Dendzik, F. Andreatta, S. S. Grønborg, I. Marković, J. M. Riley, J. C. Johannsen, D. Lizzit, L. Bignardi, S. Lizzit, C. Cacho, O. Alexander, D. Matselyukh, A. S. Wyatt, R. T. Chapman, E. Springate, J. V. Lauritsen, P. D. C. King, C. E. Sanders, J. A. Miwa, P. Hofmann, and S. Ulstrup, Spectroscopic view of ultrafast charge carrier dynamics in single- and bilayer transition metal dichalcogenide semiconductors, J. Electron Spectrosc. Relat. Phenom. 250, 147093 (2021).
  43. V. Smejkal, F. Libisch, A. Molina-Sanchez, C. Trovatello, L. Wirtz, and A. Marini, Time-dependent screening explains the ultrafast excitonic signal rise in 2D semiconductors, ACS Nano 15, 1179 (2021).
  44. J. Kang, W. Liu, D. Sarkar, D. Jena, and K. Banerjee, Computational study of metal contacts to monolayer transition-metal dichalcogenide semiconductors, Phys. Rev. X 4, 031005 (2014).
  45. H. Lee, S. Deshmukh, J. Wen, V. Z. Costa, J. S. Schuder, M. Sanchez, A. S. Ichimura, E. Pop, B. Wang, and A. K. M. Newaz, Layer-dependent interfacial transport and optoelectrical properties of MoS2 on ultraflat metals, ACS Appl. Mater. Interfaces 11, 31543 (2019).
  46. E. Pollmann, S. Sleziona, T. Foller, U. Hagemann, C. Gorynski, O. Petri, L. Madauß, L. Breuer, and M. Schleberger, Large-Area, Two-dimensional MoS2 exfoliated on gold: Direct experimental access to the metal–semiconductor interface, ACS Omega 6, 15929 (2021).
  47. S. I. Anisimov, B. L. Kapeliovich, and T. L. Perel'man, Electron emission from metal surfaces exposed to ultrashort laser pulses, Sov. Phys. JETP 39, 375 (1974).
  48. H. Wang, C. Zhang, and F. Rana, Ultrafast dynamics of defect-assisted electron–hole recombination in monolayer MoS2, Nano Lett. 15, 339 (2015).
  49. H.-P. Komsa and A. V. Krasheninnikov, Native defects in bulk and monolayer MoS2 from first principles, Phys. Rev. B 91, 125304 (2015).
  50. B. Schuler, D. Y. Qiu, S. Refaely-Abramson, C. Kastl, C. T. Chen, S. Barja, R. J. Koch, D. F. Ogletree, S. Aloni, A. M. Schwartzberg, J. B. Neaton, S. G. Louie, and A. Weber-Bargioni, Large spin-orbit splitting of deep in-gap defect states of engineered sulfur vacancies in monolayer WS2, Phys. Rev. Lett. 123, 076801 (2019).
  51. R. Krause, S. Aeschlimann, M. Chávez-Cervantes, R. Perea-Causin, S. Brem, E. Malic, S. Forti, F. Fabbri, C. Coletti, and I. Gierz, Microscopic understanding of ultrafast charge transfer in van der Waals heterostructures, Phys. Rev. Lett. 127, 276401 (2021).
  52. A. Bruix, J. A. Miwa, N. Hauptmann, D. Wegner, S. Ulstrup, S. S. Grønborg, C. E. Sanders, M. Dendzik, A. G. Čabo, M. Bianchi, J. V. Lauritsen, A. A. Khajetoorians, B. Hammer, and P. Hofmann, Single-layer MoS2 on Au(111): Band gap renormalization and substrate interaction, Phys. Rev. B 93, 165422 (2016).
  53. D. M. Newns, Self-consistent model of hydrogen chemisorption, Phys. Rev. 178, 1123 (1969).

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