Electron Spin Decoherence Dynamics in Magnetic Manganese Hybrid Organic-Inorganic Crystals: The Effect of Lattice Dimensionality

Zheng，Haining1,2; Ghosh，Arup3; Swamynadhan，M. J.4; Wang，Gang5; Zhang，Qihan6; Wu，Xiao2; Abdelwahab，Ibrahim2; Wong，Walter P.D.2; Xu，Qing Hua2; Ghosh，Saurabh4; Chen，Jingsheng6; Campbell，Branton J.7; Stroppa，Alessandro8; Lin，Junhao5,9; Mahendiran，Ramanathan3; Loh，Kian Ping1,2

2023

10.1021/jacs.3c05503

Journal of the American Chemical Society   Impact Factor & Quartile

0002-7863

1520-5126

Organic-inorganic metal hybrids with their tailorable lattice dimensionality and intrinsic spin-splitting properties are interesting material platforms for spintronic applications. While the spin decoherence process is extensively studied in lead- and tin-based hybrids, these systems generally show short spin decoherence lifetimes, and their correlation with the lattice framework is still not well-understood. Herein, we synthesized magnetic manganese hybrid single crystals of (4-fluorobenzylamine)MnCl, ((R)-3-fluoropyrrolidinium)MnCl, and (pyrrolidinium)MnCl, which represent a change in lattice dimensionality from 2D and 1D to 0D, and studied their spin decoherence processes using continuous-wave electron spin resonance spectroscopy. All manganese hybrids exhibit nanosecond-scale spin decoherence time τ dominated by the symmetry-directed spin exchange interaction strengths of Mn-Mn pairs, which is much longer than lead- and tin-based metal hybrids. In contrast to the similar temperature variation laws of τ in 2D and 0D structures, which first increase and gradually drop afterward, the 1D structure presents a monotonous rise of τ with the temperatures, indicating the strong correlation of spin decoherence with the lattice rigidity of the inorganic framework. This is also rationalized on the basis that the spin decoherence is governed by the competitive contributions from motional narrowing (prolonging the τ) and electron-phonon coupling interaction (shortening the τ), both of which are thermally activated, with the difference that the former is more pronounced in rigid crystalline lattices.

SCI

English

NI Journal Papers

Corresponding

Singapore's National Research Foundation[NRF CRP22-2019-0006] ; Ministry of Education[A-0004212-00-00] ; National Natural Science Foundation of China[11974156] ; Guangdong Innovative and Entrepreneurial Research Team Program[2019ZT08C044] ; Shenzhen Science and Technology Program["KQTD20190929173815000","20200925161102001"] ; Science, Technology, and Innovation Commission of Shenzhen Municipality[ZDSYS20190902092905285] ; null[ECS00000041]

Chemistry

Chemistry, Multidisciplinary

WOS:001048175900001

AMER CHEMICAL SOC

2-s2.0-85168787754

Scopus

1.Joint School of National University of Singapore and Tianjin University,Fuzhou,International Campus of Tianjin University, Binhai New City,350207,China
2.Department of Chemistry,National University of Singapore,3 Science Drive 3,117543,Singapore
3.Department of Physics,National University of Singapore,2 Science Drive 3,117551,Singapore
4.Department of Physics and Nanotechnology,SRM Institute of Science and Technology,Kattankulathur,Tamil Nadu,603203,India
5.Department of Physics and Shenzhen Key Laboratory of Advanced Quantum Functional Materials and Devices,Southern University of Science and Technology,Shenzhen,518055,China
6.Department of Materials Science and Engineering,National University of Singapore,117575,Singapore
7.Department of Physics & Astronomy,Brigham Young University,Provo,84602,United States
8.Consiglio Nazionale delle Ricerche,Institute for Superconducting and Innovative Materials and Devices (CNR-SPIN),Department of Physical and Chemical Sciences,University of L’Aquila,Coppito,Via Vetoio, L’Aquila,I-67100,Italy
9.Quantum Science Center of Guangdong−Hong Kong−Macao Greater Bay Area (Guangdong),Shenzhen,518045,China

Zheng，Haining,Ghosh，Arup,Swamynadhan，M. J.,et al. Electron Spin Decoherence Dynamics in Magnetic Manganese Hybrid Organic-Inorganic Crystals: The Effect of Lattice Dimensionality[J]. Journal of the American Chemical Society,2023.

Zheng，Haining.,Ghosh，Arup.,Swamynadhan，M. J..,Wang，Gang.,Zhang，Qihan.,...&Loh，Kian Ping.(2023).Electron Spin Decoherence Dynamics in Magnetic Manganese Hybrid Organic-Inorganic Crystals: The Effect of Lattice Dimensionality.Journal of the American Chemical Society.

Zheng，Haining,et al."Electron Spin Decoherence Dynamics in Magnetic Manganese Hybrid Organic-Inorganic Crystals: The Effect of Lattice Dimensionality".Journal of the American Chemical Society (2023).