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From interface-limited to Auger-dominated carrier dynamics in π-SnS

Laurell, Hugo LU ; Xiong, Kevin ; Ouahioune, Nedjma LU orcid ; Kjellberg Jensen, Thomas LU orcid ; Adelman, Jonah R. ; Gannan, Kylie J. ; Quintero-Bermudez, Rafael ; Verbitsky, Lior ; Le, Han K.D. and Mikkelsen, Anders LU , et al. (2026) In arXiv.org
Abstract
Metastable cubic tin(II) sulfide (π-SnS) is an earth-abundant semiconductor whose three-dimensionally bonded chiral lattice may overcome the short minority-carrier lifetime of orthorhombic SnS while maintaining a near-ideal bandgap for tandem photovoltaics. Despite its promise, ultrafast carrier cooling and recombination mechanisms over illumination density remain poorly constrained. We use core-level extreme-ultraviolet attosecond transient absorption spectroscopy at the Sn 4d edge to track carrier injection, cooling, and recombination in π-SnS with element- and orbital-specific sensitivity. Following femtosecond near-infrared excitation, the Sn 4d→CB onset exhibits conduction-band state filling and a carrier-induced edge shift, enabling... (More)
Metastable cubic tin(II) sulfide (π-SnS) is an earth-abundant semiconductor whose three-dimensionally bonded chiral lattice may overcome the short minority-carrier lifetime of orthorhombic SnS while maintaining a near-ideal bandgap for tandem photovoltaics. Despite its promise, ultrafast carrier cooling and recombination mechanisms over illumination density remain poorly constrained. We use core-level extreme-ultraviolet attosecond transient absorption spectroscopy at the Sn 4d edge to track carrier injection, cooling, and recombination in π-SnS with element- and orbital-specific sensitivity. Following femtosecond near-infrared excitation, the Sn 4d→CB onset exhibits conduction-band state filling and a carrier-induced edge shift, enabling extraction of density-dependent kinetics. The transient response follows a biexponential decay with a fast hot-carrier cooling component and a slower recombination component. At low carrier densities, recombination is consistent with interface-limited processes, whereas above ∼1x1020 cm-3 both cooling and recombination accelerate, indicating a crossover to carrier-carrier interaction-dominated dynamics. Coherent phonon oscillations with a period of∼188 fs reveal coupling between electronic excitation and lattice motion. These results provide a comprehensive picture of nonequilibrium carrier and phonon dynamics in cubic SnS, reveal a change of mechanisms over a range of carrier densities, and establish the value of using attosecond transient absorption spectroscopy to study ultrafast processes in complex semiconductors that have optoelectronic and energy-conversion applications. (Less)
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organization
publishing date
type
Working paper/Preprint
publication status
published
subject
in
arXiv.org
publisher
arXiv.org
ISSN
2331-8422
DOI
10.48550/arXiv.2602.13886
language
English
LU publication?
yes
id
cf228ff7-7927-45d0-9d75-0370dc487b50
date added to LUP
2026-06-04 16:05:11
date last changed
2026-06-06 03:31:07
@misc{cf228ff7-7927-45d0-9d75-0370dc487b50,
  abstract     = {{Metastable cubic tin(II) sulfide (π-SnS) is an earth-abundant semiconductor whose three-dimensionally bonded chiral lattice may overcome the short minority-carrier lifetime of orthorhombic SnS while maintaining a near-ideal bandgap for tandem photovoltaics. Despite its promise, ultrafast carrier cooling and recombination mechanisms over illumination density remain poorly constrained. We use core-level extreme-ultraviolet attosecond transient absorption spectroscopy at the Sn 4d edge to track carrier injection, cooling, and recombination in π-SnS with element- and orbital-specific sensitivity. Following femtosecond near-infrared excitation, the Sn 4d→CB onset exhibits conduction-band state filling and a carrier-induced edge shift, enabling extraction of density-dependent kinetics. The transient response follows a biexponential decay with a fast hot-carrier cooling component and a slower recombination component. At low carrier densities, recombination is consistent with interface-limited processes, whereas above ∼1x10<sup>20</sup> cm<sup>-3</sup> both cooling and recombination accelerate, indicating a crossover to carrier-carrier interaction-dominated dynamics. Coherent phonon oscillations with a period of∼188 fs reveal coupling between electronic excitation and lattice motion. These results provide a comprehensive picture of nonequilibrium carrier and phonon dynamics in cubic SnS, reveal a change of mechanisms over a range of carrier densities, and establish the value of using attosecond transient absorption spectroscopy to study ultrafast processes in complex semiconductors that have optoelectronic and energy-conversion applications.}},
  author       = {{Laurell, Hugo and Xiong, Kevin and Ouahioune, Nedjma and Kjellberg Jensen, Thomas and Adelman, Jonah R. and Gannan, Kylie J. and Quintero-Bermudez, Rafael and Verbitsky, Lior and Le, Han K.D. and Mikkelsen, Anders and Yang, Peidong and Hägglund, Carl and Leone, Stephen R.}},
  issn         = {{2331-8422}},
  language     = {{eng}},
  note         = {{Preprint}},
  publisher    = {{arXiv.org}},
  series       = {{arXiv.org}},
  title        = {{From interface-limited to Auger-dominated carrier dynamics in π-SnS}},
  url          = {{http://dx.doi.org/10.48550/arXiv.2602.13886}},
  doi          = {{10.48550/arXiv.2602.13886}},
  year         = {{2026}},
}