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Energy-Resolved Ultrafast Spectroscopic Investigation on the Spin-Coupled Electronic States in Multiferroic Hexagonal HoMnO₃.

ABSTRACT: A complete temperature-dependent scheme of the Mn³⁺ on-site d-d transitions in multiferroic hexagonal HoMnO₃ (h-HoMnO₃) thin films was unveiled by energy-resolved ultrafast spectroscopy. The results unambiguously revealed that the ultrafast responses of the e_1g and e_2g states differed significantly in the hexagonal HoMnO₃. We demonstrated that the short-range antiferromagnetic and ferroelectric orderings are more relevant to the e_2g state, whereas the long-range antiferromagnetic ordering is intimately coupled to both the e_2g and e_1g states. Moreover, the primary thermalization times of the e_2g and e_1g states were 0.34 ± 0.08 ps and 0.38 ± 0.08 ps, respectively.

SUBMITTER: Huang WH

PROVIDER: S-EPMC9332413 | biostudies-literature | 2022 Jul

REPOSITORIES: biostudies-literature

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Energy-Resolved Ultrafast Spectroscopic Investigation on the Spin-Coupled Electronic States in Multiferroic Hexagonal HoMnO3.

Huang Wei-Hong WH Wei Hao-Keng HK Quyen Nguyen Nhat NN Yang Pei-Tsung PT Cheng Yi-Cheng YC Wang Yu-Ting YT Ko Ying-Kuan YK Tu Chien-Ming CM Yabushita Atsushi A Luo Chih-Wei CW

Materials (Basel, Switzerland) 20220726 15

A complete temperature-dependent scheme of the Mn3+ on-site d-d transitions in multiferroic hexagonal HoMnO3 (h-HoMnO3) thin films was unveiled by energy-resolved ultrafast spectroscopy. The results unambiguously revealed that the ultrafast responses of the e1g and e2g states differed significantly in the hexagonal HoMnO3. We demonstrated that the short-range antiferromagnetic and ferroelectric orderings are m ...[more]

PMID: 35897619

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Project description:Physisorption on hexagonal boron nitride (hBN) gained interest over the years thanks to its properties (chemically and thermally stable, insulating properties, etc.) and similarities to the well-known graphene. A recent study showed flat-on adsorption of several cationic thiacarbocyanine dyes on hBN with a tendency to form weakly coupled H- or I-type aggregates, while a zwitterionic thiacarbocyanine dye rather led to a tilted adsorption. With this in-depth time-resolved study using the TC-SPC technique, we confirm the results proven by adsorption isotherms, atomic force microscopy, and stationary state spectroscopy combined with molecular mechanics simulations and estimation of the corresponding exciton interaction. The absence of a systematic trend for the dependence of the decay times, normalized amplitudes of the decay components, and contribution of different components to the stationary emission spectra upon the emission wavelength observed for all studied dyes and coverages suggests the occurrence of a single emitting species. At low coverage levels, the non-mono-exponential character of the decays was attributed to adsorption on different sites characterized by different intramolecular rotational freedom or energy transfer to nonfluorescent traps or a combination of both. The difference between the decay rates of the four dyes reflects a different density of the nonfluorescent traps. Although the decay time of the unquenched dyes was in the order of magnitude of that of dye monomers in a rigid environment, it is also compatible with weakly coupled aggregates such as proposed earlier based on the stationary spectra. Hence, the adsorption leads to a rigid environment of the dyes, blocking internal conversion. Increasing the concentration of the dye solution from which the adsorption on hBN occurs increases not only the coverage of the hBN surface but also the extent of energy transfer to nonfluorescent traps. For TDC (5,5-dichloro-3-3'-diethyl-9-ethyl-thiacarbocyanine) and TD2 (3-3'-diethyl-9-ethyl-thiacarbocyanine), besides direct energy transfer to traps, exciton hopping between dye dimers followed by energy transfer to these traps occurs, which resulted in a decreasing decay time of the longest decaying component. For all dyes, it was also possible to analyze the fluorescence decays as a stretched exponential as would be expected for energy transfer to randomly distributed traps in a two-dimensional (2D) geometry. This analysis yielded a fluorescence decay time of the unquenched dyes similar to the longest decay time obtained by analysis of the fluorescence decays as a sum of three of four exponentials.

Dataset Information

Energy-Resolved Ultrafast Spectroscopic Investigation on the Spin-Coupled Electronic States in Multiferroic Hexagonal HoMnO₃.

Publications

Energy-Resolved Ultrafast Spectroscopic Investigation on the Spin-Coupled Electronic States in Multiferroic Hexagonal HoMnO<sub>3</sub>.

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