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  Exciton control in a room temperature bulk semiconductor with coherent strain pulses

Baldini, E., Dominguez, A., Palmieri, T., Cannelli, O., Rubio, A., Ruello, P., et al. (2019). Exciton control in a room temperature bulk semiconductor with coherent strain pulses. Science Advances, 5(11): eaax2937. doi:10.1126/sciadv.aax2937.

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eaax2937.full.pdf (Publisher version), 451KB
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This is an open-access article distributed under the terms of the Creative Commons Attribution-NonCommercial license, which permits use, distribution, and reproduction in any medium, so long as the resultant use is not for commercial advantage and provided the original work is properly cited.
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© the Author(s), some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works.
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aax2937_SM.pdf (Supplementary material), 537KB
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Section S1. Global fit analysis Section S2. Generation mechanism Section S3. Phenomenological description of the observed exciton renormalization Section S4. Perturbative model for coherent acoustic phonons Section S5. Additional many-body perturbation theory calculations Fig. S1. Traditional approach of ultrafast acoustics applied to anatase TiO2. Fig. S2. Simulation of the transient acoustic signal. Fig. S3. Many-body perturbation theory calculations on the strained unit cell. Fig. S4. Calculation of the photoelastic coefficients. Fig. S5. Comparison between the RPA-GW and BSE-GW results.
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 Creators:
Baldini, E.1, Author
Dominguez, A.2, Author
Palmieri, T.1, Author
Cannelli, O.1, Author
Rubio, A.2, 3, 4, 5, Author           
Ruello, P.6, Author
Chergui, M.1, Author
Affiliations:
1Laboratory of Ultrafast Spectroscopy, ISIC and Lausanne Centre for Ultrafast Science (LACUS), École Polytechnique Fédérale de Lausanne (EPFL), ou_persistent22              
2Departamento Fisica de Materiales, Universidad del País Vasco, ou_persistent22              
3Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_2266715              
4Center for Free Electron Laser Science, ou_persistent22              
5Center for Computational Quantum Physics, Simons Foundation Flatiron Institute, ou_persistent22              
6Institut des Molécules et Matériaux du Mans, ou_persistent22              

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 Abstract: Controlling the excitonic optical properties of room temperature semiconductors using time-dependent perturbations is key to future optoelectronic applications. The optical Stark effect in bulk and low-dimensional materials has recently shown exciton shifts below 20 meV. Here, we demonstrate dynamical tuning of the exciton properties by photoinduced coherent acoustic phonons in the cheap and abundant wide-gap semiconductor anatase titanium dioxide (TiO2) in single crystalline form. The giant coupling between the excitons and the photoinduced strain pulses yields a room temperature exciton shift of 30 to 50 meV and a marked modulation of its oscillator strength. An advanced ab initio treatment of the exciton-phonon interaction fully accounts for these results, and shows that the deformation potential coupling underlies the generation and detection of the giant acoustic phonon modulations.

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Language(s): eng - English
 Dates: 2019-03-192019-10-082019-11-29
 Publication Status: Published online
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 Rev. Type: Peer
 Identifiers: DOI: 10.1126/sciadv.aax2937
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Project name : We acknowledge support by the Swiss NSF via the NCCR:MUST and R’EQUIP and by the European Research Council Advanced Grant DYNAMOX. This project has received funding from the European Union’s Horizon 2020 research and innovation program under Marie Sklodowska-Curie grant agreement no. 753874.
Grant ID : 753874
Funding program : Horizon 2020 (H2020)
Funding organization : European Commission (EC)

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Title: Science Advances
  Other : Sci. Adv.
Source Genre: Journal
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Publ. Info: Washington : AAAS
Pages: - Volume / Issue: 5 (11) Sequence Number: eaax2937 Start / End Page: - Identifier: ISSN: 2375-2548
CoNE: https://pure.mpg.de/cone/journals/resource/2375-2548