Optical control of a metastable phase in the charge density wave Mott insulator <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:mrow> <mml:mn>1</mml:mn> <mml:mi>T</mml:mi> <mml:mtext>−</mml:mtext> <mml:msub> <mml:mi>TaS</mml:mi> <mml:m

Light-induced metastable phases are exotic, long-lived out-of-equilibrium states of matter. Optical control offers a powerful approach to engineering these phases, enabling dynamic tuning of their electronic and structural properties. Using time- and angle-resolved photoemission spectroscopy, we investigate the emergence of a metastable phase induced by a strong infrared pump in the charge-density-wave (CDW)-Mott insulator <a:math xmlns:a="http://www.w3.org/1998/Math/MathML"> <a:mrow> <a:mn>1</a:mn> <a:mi>T</a:mi> <a:mtext>−</a:mtext> <a:msub> <a:mi>TaS</a:mi> <a:mn>2</a:mn> </a:msub> </a:mrow> </a:math> . Furthermore, we demonstrate how its properties can be optically manipulated by varying the photoexcitation strength. A long-lived stabilization of the renormalized electronic band structure serves as a signature of the metastable phase. It displays a relaxed periodic lattice distortion (PLD) and primarily lattice-driven dynamics. The emergence of a new dispersive band in the vicinity of the Hubbard bands reveals the formation of a novel band structure unique to the metastable phase. Our pump-fluence-dependent studies reveal a threshold (incident) fluence <b:math xmlns:b="http://www.w3.org/1998/Math/MathML"> <b:mrow> <b:msub> <b:mi>F</b:mi> <b:mi>C</b:mi> </b:msub> <b:mo>∼</b:mo> <b:mspace width="0.16em"/> <b:mn>1.3</b:mn> <b:mi>mJ</b:mi> <b:mo>/</b:mo> <b:msup> <b:mrow> <b:mi>cm</b:mi> </b:mrow> <b:mn>2</b:mn> </b:msup> </b:mrow> </b:math> for inducing the metastable phase, above which the band renormalization continuously evolves with increasing fluence. For <d:math xmlns:d="http://www.w3.org/1998/Math/MathML"> <d:mrow> <d:mi>F</d:mi> <d:mo>⩽</d:mo> </d:mrow> </d:math> 3.4 <e:math xmlns:e="http://www.w3.org/1998/Math/MathML"> <e:mrow> <e:mi>mJ</e:mi> <e:mo>/</e:mo> <e:msup> <e:mrow> <e:mi>cm</e:mi> </e:mrow> <e:mn>2</e:mn> </e:msup> </e:mrow> </e:math> , stronger photoexcitation progressively drives the phase to higher energies, accompanied by a more relaxed PLD and reduced CDW amplitude. The properties of the metastable phase are strongly influenced by the transient dynamics at each fluence, and the associated fast timescales suggest that the intrinsic CDW amplitude mode remains unaffected by optical manipulation. These findings highlight the potential of optical control in tuning the properties of metastable phases in quantum materials, offering new insights into the manipulation of CDW systems and paving the way for future investigations in nonequilibrium phase engineering.

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Journal
Physical review. B./Physical review. B
Published
2025-11-19
DOI
https://doi.org/10.1103/gz2s-685y
Primary Topic
2D Materials and Applications
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article
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article

Optical control of a metastable phase in the charge density wave Mott insulator <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:mrow> <mml:mn>1</mml:mn> <mml:mi>T</mml:mi> <mml:mtext>−</mml:mtext> <mml:msub> <mml:mi>TaS</mml:mi> <mml:m

Karl J. Friston
Physical review. B./Physical review. B
2D Materials and Applications
article

Optical control of a metastable phase in the charge density wave Mott insulator <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:mrow> <mml:mn>1</mml:mn> <mml:mi>T</mml:mi> <mml:mtext>−</mml:mtext> <mml:msub> <mml:mi>TaS</mml:mi> <mml:m

Karl J. Friston
article en

Abstract

Light-induced metastable phases are exotic, long-lived out-of-equilibrium states of matter. Optical control offers a powerful approach to engineering these phases, enabling dynamic tuning of their electronic and structural properties. Using time- and angle-resolved photoemission spectroscopy, we investigate the emergence of a metastable phase induced by a strong infrared pump in the charge-density-wave (CDW)-Mott insulator <a:math xmlns:a="http://www.w3.org/1998/Math/MathML"> <a:mrow> <a:mn>1</a:mn> <a:mi>T</a:mi> <a:mtext>−</a:mtext> <a:msub> <a:mi>TaS</a:mi> <a:mn>2</a:mn> </a:msub> </a:mrow> </a:math> . Furthermore, we demonstrate how its properties can be optically manipulated by varying the photoexcitation strength. A long-lived stabilization of the renormalized electronic band structure serves as a signature of the metastable phase. It displays a relaxed periodic lattice distortion (PLD) and primarily lattice-driven dynamics. The emergence of a new dispersive band in the vicinity of the Hubbard bands reveals the formation of a novel band structure unique to the metastable phase. Our pump-fluence-dependent studies reveal a threshold (incident) fluence <b:math xmlns:b="http://www.w3.org/1998/Math/MathML"> <b:mrow> <b:msub> <b:mi>F</b:mi> <b:mi>C</b:mi> </b:msub> <b:mo>∼</b:mo> <b:mspace width="0.16em"/> <b:mn>1.3</b:mn> <b:mi>mJ</b:mi> <b:mo>/</b:mo> <b:msup> <b:mrow> <b:mi>cm</b:mi> </b:mrow> <b:mn>2</b:mn> </b:msup> </b:mrow> </b:math> for inducing the metastable phase, above which the band renormalization continuously evolves with increasing fluence. For <d:math xmlns:d="http://www.w3.org/1998/Math/MathML"> <d:mrow> <d:mi>F</d:mi> <d:mo>⩽</d:mo> </d:mrow> </d:math> 3.4 <e:math xmlns:e="http://www.w3.org/1998/Math/MathML"> <e:mrow> <e:mi>mJ</e:mi> <e:mo>/</e:mo> <e:msup> <e:mrow> <e:mi>cm</e:mi> </e:mrow> <e:mn>2</e:mn> </e:msup> </e:mrow> </e:math> , stronger photoexcitation progressively drives the phase to higher energies, accompanied by a more relaxed PLD and reduced CDW amplitude. The properties of the metastable phase are strongly influenced by the transient dynamics at each fluence, and the associated fast timescales suggest that the intrinsic CDW amplitude mode remains unaffected by optical manipulation. These findings highlight the potential of optical control in tuning the properties of metastable phases in quantum materials, offering new insights into the manipulation of CDW systems and paving the way for future investigations in nonequilibrium phase engineering.

Physical review. B./Physical review. BVol. 113(3)
Tata Institute of Fundamental Research (IN), Jagiellonian University (PL), University of Nova Gorica (SI), Elettra-Sincrotrone Trieste S.C.p.A. (IT), Istituto Officina dei Materiali (IT), Center for Biomolecular Nanotechnologies (IT), University of Duisburg-Essen (DE), AGH University of Krakow (PL)
Openalex Percentile: Top 67%
2D Materials and Applications
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