Anomalous non-equilibrium response in black phosphorus to sub-gap mid-infrared excitation

Angela Montanaro, Francesca Giusti, Matteo Zanfrognini, Paola Pietro, Filippo Glerean, Giacomo Jarc, Enrico Maria Rigoni, Shahla Y. Mathengattil, Daniele Varsano, Massimo Rontani, Andrea Perucchi, Elisa Molinari and Daniele Fausti ()
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Angela Montanaro: Università degli Studi di Trieste
Francesca Giusti: Università degli Studi di Trieste
Matteo Zanfrognini: Università degli Studi di Modena e Reggio Emilia
Paola Pietro: Elettra Sincrotrone Trieste S.C.p.A.
Filippo Glerean: Università degli Studi di Trieste
Giacomo Jarc: Università degli Studi di Trieste
Enrico Maria Rigoni: Università degli Studi di Trieste
Shahla Y. Mathengattil: Università degli Studi di Trieste
Daniele Varsano: Consiglio Nazionale delle Ricerche—Istituto Nanoscienze
Massimo Rontani: Consiglio Nazionale delle Ricerche—Istituto Nanoscienze
Andrea Perucchi: Elettra Sincrotrone Trieste S.C.p.A.
Elisa Molinari: Università degli Studi di Modena e Reggio Emilia
Daniele Fausti: Università degli Studi di Trieste

Nature Communications, 2022, vol. 13, issue 1, 1-7

Abstract: Abstract The competition between the electron-hole Coulomb attraction and the 3D dielectric screening dictates the optical properties of layered semiconductors. In low-dimensional materials, the equilibrium dielectric environment can be significantly altered by the ultrafast excitation of photo-carriers, leading to renormalized band gap and exciton binding energies. Recently, black phosphorus emerged as a 2D material with strongly layer-dependent electronic properties. Here, we resolve the response of bulk black phosphorus to mid-infrared pulses tuned across the band gap. We find that, while above-gap excitation leads to a broadband light-induced transparency, sub-gap pulses drive an anomalous response, peaked at the single-layer exciton resonance. With the support of DFT calculations, we tentatively ascribe this experimental evidence to a non-adiabatic modification of the screening environment. Our work heralds the non-adiabatic optical manipulation of the electronic properties of 2D materials, which is of great relevance for the engineering of versatile van der Waals materials.

Date: 2022
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DOI: 10.1038/s41467-022-30341-4

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