Cross-examination of photoinitiated carrier and structural dynamics of black phosphorus at elevated fluences
Revived attention in black phosphorus (bP) has been tremendous in the past decade. While many photoinitiated experiments have been conducted, a cross-examination of bP's photocarrier and structural dynamics is still lacking. In this article, we provide such analysis by examining time-resolved d...
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| Published in: | The Journal of chemical physics Vol. 160; no. 12 |
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| Main Authors: | , , |
| Format: | Journal Article |
| Language: | English |
| Published: |
United States
28.03.2024
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| ISSN: | 1089-7690, 1089-7690 |
| Online Access: | Get more information |
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| Summary: | Revived attention in black phosphorus (bP) has been tremendous in the past decade. While many photoinitiated experiments have been conducted, a cross-examination of bP's photocarrier and structural dynamics is still lacking. In this article, we provide such analysis by examining time-resolved data acquired using optical transient reflectivity and reflection ultrafast electron diffraction, two complementary methods under the same experimental conditions. At elevated excitation fluences, we find that more than 90% of the photoinjected carriers are annihilated within the first picosecond (ps) and transfer their energy to phonons in a nonthermal, anisotropic fashion. Electronically, the remaining carrier density around the band edges induces a significant interaction that leads to an interlayer lattice contraction in a few ps but soon diminishes as a result of the continuing loss of carriers. Structurally, phonon-phonon scattering redistributes the energy in the lattice and results in the generation of out-of-plane coherent acoustic phonons and thermal lattice expansion. Their onset times at ∼6 ps are found to be in good agreement. Later, a thermalized quasi-equilibrium state is reached following a period of about 40-50 ps. Hence, we propose a picture with five temporal regimes for bP's photodynamics. |
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| Bibliography: | ObjectType-Article-1 SourceType-Scholarly Journals-1 ObjectType-Feature-2 content type line 23 |
| ISSN: | 1089-7690 1089-7690 |
| DOI: | 10.1063/5.0193613 |