Interlayer exciton valley polarization dynamics in large magnetic fields

Höller, Johannes; Selig, Malte; Kempf, Michael; Zipfel, Jonas; Nagler, Philipp; Katzer, Manuel; Katsch, Florian; Ballottin, Mariana V.; Mitioglu, Anatolie; Chernikov, Alexey; Christianen, Peter C. M.; Schüller, Christian; Knorr, Andreas; Korn, Tobias

doi:10.1103/physrevb.105.085303

Cited by 16 publications

(24 citation statements)

References 47 publications

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“…Substitution of the material parameters yields 75 τ res = 12 ns and 20 ns for H-type and R-type HS, which agrees with the timescales of the PL polarization saturation 61 .…”

Section: B Mechanism Of Hole Valley-magnetophonon Resonancesupporting

confidence: 72%

“…1. ILE in H-type and Rtype heterobilayers are directly distinguishable by their emission energy and spectral linewidth, even in zero-field photoluminescence (PL) spectra 61 . As Fig.…”

Section: Resultsmentioning

confidence: 99%

“…In order to achieve crystallographic alignment, well-cleaved edges of the constituent layers are aligned parallel to each other during the transfer. Further details are published elsewhere 61 .…”

Section: A Sample Preparationmentioning

confidence: 99%

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Valley-magnetophonon resonance for interlayer excitons

Smirnov¹,

Holler²,

Kempf³

et al. 2022

Preprint

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Heterobilayers consisting of MoSe2 and WSe2 monolayers can host optically bright interlayer excitons with intriguing properties such as ultralong lifetimes and pronounced circular polarization of their photoluminescence due to valley polarization, which can be induced by circularly polarized excitation or applied magnetic fields. Here, we report on the observation of an intrinsic valley-magnetophonon resonance for localized interlayer excitons promoted by invervalley hole scattering. It leads to a resonant increase of the photoluminescence polarization degree at the same field of 24.2 Tesla for H-type and R-type stacking configurations despite their vastly different excitonic energy splittings. As a microscopic mechanism of the hole intervalley scattering we identify the scattering with chiral TA phonons of MoSe2 between excitonic states mixed by the long-range electron hole exchange interaction.

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“…Substitution of the material parameters yields 75 τ res = 12 ns and 20 ns for H-type and R-type HS, which agrees with the timescales of the PL polarization saturation 61 .…”

Section: B Mechanism Of Hole Valley-magnetophonon Resonancesupporting

confidence: 72%

“…1. ILE in H-type and Rtype heterobilayers are directly distinguishable by their emission energy and spectral linewidth, even in zero-field photoluminescence (PL) spectra 61 . As Fig.…”

Section: Resultsmentioning

confidence: 99%

See 1 more Smart Citation

Valley-magnetophonon resonance for interlayer excitons

Smirnov¹,

Holler²,

Kempf³

et al. 2022

Preprint

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“…Organic molecules show highly tunable transition energies and provide large optical dipole moments as the respective excitons are of the Frenkel type [1][2][3][4][5][6][7][8][9][10][11][12]. Transition metal dichalcogenites (TMDCs) are inorganic, atomically thin semiconductors that have stimulated research in the last years: Their atomic thickness leads to a reduced screening of the Coulomb interaction and consequently to the formation of stable, bound electron hole pairs, namely Wannier type excitons, which dominate the optical properties in the vicinity of the band edge [13][14][15][16][17][18][19][20][21][22][23]. The large oscillator strength of optically bright excitons makes TMDC monolayers ideal resonant substrates for energetically tunable molecules, but also for quantum dots [24][25][26][27], NV centers [28] and plasmonic structures [29][30][31][32].…”

Section: Introductionmentioning

confidence: 99%

Impact of dark excitons on Förster-type resonant energy transfer between dye molecules and atomically thin semiconductors

et al. 2023

Self Cite

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Interfaces of dye molecules and two-dimensional transition metal dichalcogenides (TMDCs) combine strong molecular dipole excitations with high carrier mobilities in semiconductors. Förster type energy transfer is one key mechanism for the coupling between both constituents. We report microscopic calculations of a spectrally resolved Förster induced transition rate from dye molecules to a TMDC layer. Our approach is based on microscopic Bloch equations which are solved selfconsistently together with Maxwells equations. This approach allows to incorporate the dielectric environment of a TMDC semiconductor, sandwiched between donor molecules and a substrate. Our analysis reveals transfer rates in the meV range for typical dye molecules in closely stacked structures, with a non-trivial dependence of the Förster rate on the molecular transition energy resulting from unique signatures of dark, momentum forbidden TMDC excitons.

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“…Transition-metal dichalcogenides (TMDs) have been in the focus of current research due to their enhanced lightmatter and Coulomb interaction leading to a rich energy landscape of tightly bound excitons [1][2][3][4]. Stacking TMD monolayers into van der Waals heterostructures introduces spatially separated interlayer states adding another exciton species with long lifetimes and an out-of-plane dipole moment [5][6][7][8][9][10][11][12][13][14]. Recent experiments demonstrated the ultrafast charge transfer in optically excited TMD heterobilayers resulting in a formation of interlayer states on a sub-picosecond timescale [15][16][17][18][19][20].…”

mentioning

confidence: 99%

Ultrafast phonon‐driven charge transfer in van der Waals heterostructures

2022

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Van der Waals heterostructures built by vertically stacked transition metal dichalcogenides (TMDs) exhibit a rich energy landscape including interlayer and intervalley excitons. Recent experiments demonstrated an ultrafast charge transfer in TMD heterostructures. However, the nature of the charge transfer process has remained elusive. Based on a microscopic and material-realistic exciton theory, we reveal that phonon-mediated scattering via strongly hybridized intervalley excitons governs the charge transfer process that occurs on a sub-100fs timescale. We track the time-, momentum-, and energy-resolved relaxation dynamics of optically excited excitons and determine the temperature-and stacking-dependent charge transfer time for different TMD bilayers. The provided insights present a major step in microscopic understanding of the technologically important charge transfer process in van der Waals heterostructures.

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Interlayer exciton valley polarization dynamics in large magnetic fields

Cited by 16 publications

References 47 publications

Valley-magnetophonon resonance for interlayer excitons

Valley-magnetophonon resonance for interlayer excitons

Impact of dark excitons on Förster-type resonant energy transfer between dye molecules and atomically thin semiconductors

Ultrafast phonon‐driven charge transfer in van der Waals heterostructures

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