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Exciton and trion dynamics in atomically thin MoSe2 and WSe2: Effect of localization

T. Godde, D. Schmidt, J. Schmutzler, M. Aßmann, J. Debus, F. Withers, E. M. Alexeev, O. Del Pozo-Zamudio, O. V. Skrypka, K. S. Novoselov, M. Bayer, and A. I. Tartakovskii
Phys. Rev. B 94, 165301 – Published 5 October 2016

Abstract

We present a detailed investigation of the exciton and trion dynamics in naturally doped MoSe2 and WSe2 single atomic layers as a function of temperature in the range 10–300 K under above band-gap laser excitation. By combining time-integrated and time-resolved photoluminescence (PL) spectroscopy, we show the importance of exciton and trion localization in both materials at low temperatures. We also reveal the transition to delocalized exciton complexes at higher temperatures where the exciton and trion thermal energy exceeds the typical localization energy. This is accompanied by strong changes in PL including suppression of the trion PL and decrease of the trion PL lifetime, as well as significant changes for neutral excitons in the temperature dependence of the PL intensity and the appearance of a pronounced slow PL decay component. In MoSe2 and WSe2 studied here, the temperatures where such strong changes occur are observed at around 100 and 200 K, respectively, in agreement with their inhomogeneous PL linewidth of 8 and 20 meV at T10K. The observed behavior is a result of a complex interplay between influences of the specific energy ordering of bright and dark excitons in MoSe2 and WSe2, sample doping, trion, and exciton localization and various temperature-dependent nonradiative processes.

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  • Received 19 August 2016

DOI:https://doi.org/10.1103/PhysRevB.94.165301

©2016 American Physical Society

Physics Subject Headings (PhySH)

Condensed Matter, Materials & Applied Physics

Authors & Affiliations

T. Godde1, D. Schmidt2, J. Schmutzler2, M. Aßmann2, J. Debus2, F. Withers3, E. M. Alexeev1, O. Del Pozo-Zamudio1, O. V. Skrypka1, K. S. Novoselov3, M. Bayer2, and A. I. Tartakovskii1

  • 1Department of Physics and Astronomy, University of Sheffield, Sheffield S3 7RH, United Kingdom
  • 2Experimentelle Physik 2, Technische Universität Dortmund, D-44221 Dortmund, Germany
  • 3School of Physics and Astronomy, University of Manchester, Manchester M13 9PL, United Kingdom

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Issue

Vol. 94, Iss. 16 — 15 October 2016

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Images

  • Figure 1
    Figure 1

    Time-integrated (TI) and time-resolved (TR) photoluminescence (PL) for single-monolayer MoSe2 samples. (a) TIPL spectra in the range 12–110 K. Exciton (X) and trion (X*) peaks are labeled. Spectra are multiplied by factors shown on the graph. (b) TRPL PL traces for T=12 K for X (squares) and X* (circles) (sample 1). Lines show the fitting functions. The inset shows the X PL decay time and X* rise time as a function of gate voltage in sample 5. The gate voltage is used to vary the carrier concentration in the film with a positive voltage corresponding to a higher concentration. (c) and (d) TRPL traces for X* (sample 1) in (c) and X (sample 2) in (d) for a range of temperatures. Normalized PL intensities are shown.

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  • Figure 2
    Figure 2

    Temperature dependence of time-integrated (TI) and time-resolved (TR) photoluminescence (PL) for single-monolayer MoSe2 samples. (a) Spectrally integrated TIPL intensity. Dependencies for X (squares) and X* (circles) are shown for samples 1 and 2. (b) X (squares) and X* (circles) PL decay times in samples 1 (solid symbols) and 2 (open symbols). The horizontal lines mark the setup resolution for the two experiments: the dashed line is for the 12 ps resolution corresponding to the data shown with the open symbols; the solid line is for 4 ps resolution corresponding to the data shown with the solid symbols. (c) The ratio of the time integral of the function used to fit the slow PL decay component, Islow, and the total integral under the PL decay curve, Itot, r=Islow/Itot.

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  • Figure 3
    Figure 3

    Time-integrated (TI) and time-resolved (TR) photoluminescence (PL) for single-monolayer WSe2 samples. (a) A TIPL spectrum measured at T=9 K in sample 4. Neutral exciton (X) and trion (X*) peaks as well as localized exciton peaks P1, P2, and P3 are labeled. (b) TIPL in a temperature range 9–293 K. Individual spectra at each temperature are normalized. Features as in graph (a) are labeled. (c) and (d) TRPL traces for X (c) and X* (d) in sample 3 for a range of temperatures. Normalized PL intensities are shown.

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  • Figure 4
    Figure 4

    Temperature dependence of time-integrated (TI) and time-resolved (TR) photoluminescence (PL) for single-monolayer WSe2 samples. (a) Spectrally integrated TIPL intensity. Dependencies for X (squares) and all PL in the range shown in Fig. 3 (triangles) are shown. (b),(c) X (squares) and X* (circles) PL decay times. The data for the slow and fast decay components are shown in (b) and (c), respectively. Open and solid symbols show X PL decay data for two different samples. (d) The ratio of the time integral of the function used to fit the slow PL decay component, Islow, and the total integral under the PL decay curve, Itot, r=Islow/Itot. Data for both X (squares) and X* (circles) are shown.

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