Ultrafast Dynamics of Spin-Orbit Entangled Excitons Coupled to Magnetic Ordering in van der Waals Antiferromagnet NiPS3

Fuente: arXiv
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Autori principali: Sahu, Sidhanta, Chauhan, Anupama, Ghosh, Poulami, Routh, Sayan, Puranik, Ruturaj, Thirupathaiah, Setti, Lal, Siddhartha, S, Shriganesh Prabhu, Mitra, Chiranjib, Kamaraju, N.
Natura: Preprint
Pubblicazione: 2025
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author Sahu, Sidhanta
Chauhan, Anupama
Ghosh, Poulami
Routh, Sayan
Puranik, Ruturaj
Thirupathaiah, Setti
Lal, Siddhartha
S, Shriganesh Prabhu
Mitra, Chiranjib
Kamaraju, N.
author_facet Sahu, Sidhanta
Chauhan, Anupama
Ghosh, Poulami
Routh, Sayan
Puranik, Ruturaj
Thirupathaiah, Setti
Lal, Siddhartha
S, Shriganesh Prabhu
Mitra, Chiranjib
Kamaraju, N.
contents Spin-orbit entangled excitons (SOEE) in two-dimensional (2D) antiferromagnets provide direct access to explore unconventional many body interactions in correlated electron systems. In this work, we carry out a detailed investigation using non-degenerate isotropic and anisotropic pump-probe reflection spectroscopy to probe the ultrafast dynamics of SOEE and their coupling to spin fluctuations in NiPS3. Transient reflectivity data reveals acoustic phonon oscillations at ~ 27 GHz, along with two distinct relaxation timescales: fast (1-9 ps) and slower components (1-4 ns) associated with SOEE coherence and spin reordering, respectively. Both timescales exhibit pronounced temperature dependence near the exciton dissociation (TED = 120 K) and Neel (TN = 155 K) temperatures. The SOEE coherence shortens from ~ 8-9 ps at T < TED to ~ 3 ps at T > TED with a finite tail persisting beyond TN. The spin reordering time grows near 120 K, and shows critical slowing down around TN. Pump fluence studies further corroborate their spin origin. Our findings uncover the direct interplay between the excitonic and spin degrees of freedom across ultrafast and longer timescales, offering new opportunities to probe and engineer emergent many-body interactions in 2D antiferromagnets.
format Preprint
id arxiv_https___arxiv_org_abs_2509_04900
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Ultrafast Dynamics of Spin-Orbit Entangled Excitons Coupled to Magnetic Ordering in van der Waals Antiferromagnet NiPS3
Sahu, Sidhanta
Chauhan, Anupama
Ghosh, Poulami
Routh, Sayan
Puranik, Ruturaj
Thirupathaiah, Setti
Lal, Siddhartha
S, Shriganesh Prabhu
Mitra, Chiranjib
Kamaraju, N.
Other Condensed Matter
Strongly Correlated Electrons
Spin-orbit entangled excitons (SOEE) in two-dimensional (2D) antiferromagnets provide direct access to explore unconventional many body interactions in correlated electron systems. In this work, we carry out a detailed investigation using non-degenerate isotropic and anisotropic pump-probe reflection spectroscopy to probe the ultrafast dynamics of SOEE and their coupling to spin fluctuations in NiPS3. Transient reflectivity data reveals acoustic phonon oscillations at ~ 27 GHz, along with two distinct relaxation timescales: fast (1-9 ps) and slower components (1-4 ns) associated with SOEE coherence and spin reordering, respectively. Both timescales exhibit pronounced temperature dependence near the exciton dissociation (TED = 120 K) and Neel (TN = 155 K) temperatures. The SOEE coherence shortens from ~ 8-9 ps at T < TED to ~ 3 ps at T > TED with a finite tail persisting beyond TN. The spin reordering time grows near 120 K, and shows critical slowing down around TN. Pump fluence studies further corroborate their spin origin. Our findings uncover the direct interplay between the excitonic and spin degrees of freedom across ultrafast and longer timescales, offering new opportunities to probe and engineer emergent many-body interactions in 2D antiferromagnets.
title Ultrafast Dynamics of Spin-Orbit Entangled Excitons Coupled to Magnetic Ordering in van der Waals Antiferromagnet NiPS3
topic Other Condensed Matter
Strongly Correlated Electrons
url https://arxiv.org/abs/2509.04900