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泵浦分子磁体的时间演化——一项时间分辨非弹性中子散射研究

Time evolution of a pumped molecular magnet-A time-resolved inelastic neutron scattering study.

作者信息

Reeder T R, Titum Paraj, Kindervater J, Stewart V J, Ye Q, Rodriguez-Rivera J A, Qiu Y, Maliszewskyj N, McQueen T M, Broholm C L

机构信息

William H. Miller III Department of Physics and Astronomy, The Johns Hopkins University, Baltimore, MD 21218.

Research and Exploratory Development, Johns Hopkins University Applied Physics Laboratory, Laurel, MD 20723.

出版信息

Proc Natl Acad Sci U S A. 2025 Jan 7;122(1):e2415300121. doi: 10.1073/pnas.2415300121. Epub 2025 Jan 2.

DOI:10.1073/pnas.2415300121
PMID:39746040
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11725827/
Abstract

Introducing an experimental technique of time-resolved inelastic neutron scattering (TRINS), we explore the time-dependent effects of resonant pulsed microwaves on the molecular magnet CrFPiv. The octagonal rings of magnetic Cr atoms with antiferromagnetic interactions form a singlet ground state with a weakly split triplet of excitations at 0.8 meV. A 4.6 tesla field was applied to tune the splitting between two members of the triplet excited level [Formula: see text] to resonance with 105 GHz (0.434 meV) microwaves. The time-dependent occupations of the ground state [Formula: see text], lower lying levels [Formula: see text] and [Formula: see text], and higher energy states [Formula: see text] were extracted during and after 20 s long microwave pulses incident along the (101) direction of a CrFPiv crystal held at 1.9 K. At significantly elevated spin temperatures, we found underpopulation relative to thermal equilibrium of [Formula: see text] and spin-lattice thermalization time scales ranging from 1.6(2) s to 5.7(2) s depending on the power level. This contrasts with the relaxation time [Formula: see text]s inferred for [Formula: see text] from in situ Electron Spin Resonance measurements. By probing a broad range of excited states during intense microwave pumping, TRINS thus provides a first view of long lived excited states in a molecular antiferromagnet.

摘要

我们介绍了一种时间分辨非弹性中子散射（TRINS）实验技术，以此探究共振脉冲微波对分子磁体CrFPiv的时间相关效应。具有反铁磁相互作用的磁性Cr原子八边形环形成一个单重基态，在0.8毫电子伏特处有一个微弱分裂的三重激发态。施加4.6特斯拉的磁场，以调节三重激发态[公式：见原文]的两个成员之间的分裂，使其与105吉赫兹（0.434毫电子伏特）的微波共振。在沿着保持在1.9 K的CrFPiv晶体的（101）方向入射20秒长的微波脉冲期间及之后，提取了基态[公式：见原文]、较低能级[公式：见原文]和[公式：见原文]以及较高能态[公式：见原文]的时间相关占据情况。在显著升高的自旋温度下，我们发现相对于热平衡，[公式：见原文]的粒子数不足，并且自旋 - 晶格热化时间尺度在1.6(2)秒到5.7(2)秒之间，这取决于功率水平。这与从原位电子自旋共振测量推断出的[公式：见原文]的弛豫时间[公式：见原文]秒形成对比。通过在强微波泵浦期间探测广泛的激发态，TRINS因此首次展现了分子反铁磁体中长寿命激发态的情况。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/40ba/11725827/15a4eef760c0/pnas.2415300121fig08.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/40ba/11725827/482c3b636a77/pnas.2415300121fig01.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/40ba/11725827/86eb5a14941a/pnas.2415300121fig02.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/40ba/11725827/b7da70bb2d23/pnas.2415300121fig03.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/40ba/11725827/fe849e0a25e3/pnas.2415300121fig04.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/40ba/11725827/97672e78373d/pnas.2415300121fig05.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/40ba/11725827/617c047d0afb/pnas.2415300121fig06.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/40ba/11725827/2fc694c4bb8b/pnas.2415300121fig07.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/40ba/11725827/15a4eef760c0/pnas.2415300121fig08.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/40ba/11725827/482c3b636a77/pnas.2415300121fig01.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/40ba/11725827/86eb5a14941a/pnas.2415300121fig02.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/40ba/11725827/b7da70bb2d23/pnas.2415300121fig03.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/40ba/11725827/fe849e0a25e3/pnas.2415300121fig04.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/40ba/11725827/97672e78373d/pnas.2415300121fig05.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/40ba/11725827/617c047d0afb/pnas.2415300121fig06.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/40ba/11725827/2fc694c4bb8b/pnas.2415300121fig07.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/40ba/11725827/15a4eef760c0/pnas.2415300121fig08.jpg

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