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Review

Molecular Nanomagnets with Photomagnetic Properties: Design Strategies and Recent Advances

by
Xiaoshuang Gou
1,2,
Xinyu Sun
1,
Peng Cheng
1,* and
Wei Shi
1,*
1
Frontiers Science Center for New Organic Matter, State Key Laboratory of Advanced Chemical Power Sources and Department of Chemistry, College of Chemistry, Nankai University, Tianjin 300071, China
2
i-Lab, Suzhou Institute of Nano-Tech and Nano-Bionics (SINANO), Chinese Academy of Sciences (CAS), Suzhou 215123, China
*
Authors to whom correspondence should be addressed.
Magnetochemistry 2025, 11(9), 77; https://doi.org/10.3390/magnetochemistry11090077
Submission received: 21 July 2025 / Revised: 27 August 2025 / Accepted: 28 August 2025 / Published: 31 August 2025
(This article belongs to the Special Issue Molecular Magnetism: A Themed Issue in Honor of Professor Dai-Zheng Liao on the Occasion of His 85th Birthday)
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Abstract

The magnetic properties of molecular nanomagnets can be finely modulated by light, which provides great potential in optical switches, smart sensors, and data storage devices. Light-induced spin transition, structure changes, and radical formation could tune the static and dynamic magnetic properties of molecular nanomagnets with high spatial and temporal resolutions. Herein, we summarize the design strategies of photoresponsive molecular nanomagnets and review the recent advances in transition metal/lanthanide molecular nanomagnets with photomagnetic properties. The photoresponsive mechanism based on spin transition, photocyclization, and photogenerated radicals is discussed in detail, providing insights into the photomagnetic properties of molecular nanomagnets for advanced photoresponsive materials.

1. Introduction

Stimuli-responsive materials have recently garnered great attention due to their physical and chemical properties being modulated by external stimuli, such as temperature, electric field, and light [1,2,3,4]. Among the diverse stimuli-responsive materials, photoresponsive molecular nanomagnets are particularly intriguing candidates, showing great potential toward applications such as high-density information storage, optical switching devices, smart sensors, and spintronic devices [5,6,7,8].
Molecular nanomagnets, including single-molecule magnets (SMMs) and single-chain magnets (SCMs), are usually constructed by magnetically anisotropic transition or lanthanide metal centers and organic ligands [9,10,11]. The electronic state of metal ions that is defined by the coordination sphere is crucial for the rational design of advanced molecular nanomagnets possessing tailored photomagnetic properties [12,13,14]. For example, photomagnetic properties were observed in cyanide-bridged spin-crossover (SCO) complexes with the light-induced excited spin state trapping (LIESST) effect. The LIESST effect was also applied to modulate the bistable states of molecular nanomagnets, such as {[W(CN)8][(FeII)(bib)2](bibH)}·2CH3OH (bib = 1,4-bis(1H-imidazol-1-yl)benzene), representing an example of reversible switching between SCM and SMM behaviors via light [15]. On the other hand, lanthanide SMMs have been extensively studied, achieving groundbreaking progress, especially in effective energy barrier (Ueff) and blocking temperature (TB) [16,17,18,19,20,21,22,23]. Early studies have demonstrated that light irradiation can effectively modulate the static magnetic susceptibility of lanthanide SMMs; however, regulating their dynamic magnetic susceptibility remains challenging [24,25,26]. Selected examples of photoresponsive lanthanide SMMs generally have photoresponsive cyclic units, such as 1,2-bis(4-pyridyl)ethylene [27], 9-diethylphosphorylmethylanthracene [28], and dipyridyldithienylethene [29], as well as photoresponsive radical precursors [30]. To gain insights into the mechanism of photomagnetic properties of molecular nanomagnets, we summarize the advancements of transition metal and lanthanide molecular nanomagnets with static and dynamic magnetic properties modulated by light (Figure 1). The roles of selecting organic ligands that can undergo light-induced ring-opening/ring-closing transitions or generate stable radicals under illumination are discussed, providing key structural factors for the rational design and synthesis of high-performance lanthanide molecular nanomagnets with photoinduced magnetic prop-erties.

2. Design Strategies for Molecular Nanomagnets with Photomagnetic Properties

Molecular nanomagnets with photomagnetic properties are primarily synthesized by introducing photoresponsive components, notably SCO units, photo-isomerizing organics, or radical-forming moieties. In transition metal molecular nanomagnets, incorporation of SCO units could facilitate optical switching of spin states to modulate the magnetic properties of SMMs and SCMs [31,32,33,34]. For lanthanide molecular nanomagnets, light-induced ligand transformations such as photocyclization or radical formation could modify the ligand field of the metal center and introduce additional spin carriers, thereby tuning room-temperature magnetic moments and/or dynamic magnetic susceptibilities [27,28,29,30].

2.1. Photoresponsive Spin-Crossover Units

The photoinduced electron transfer is fundamental in photophysics and photochemistry, with extensive applications in artificial light sources, solar energy conversion, and photocatalysis [35,36,37,38,39,40,41,42,43,44,45,46,47,48,49], enabling the regulation of properties at a molecular level [50,51,52]. SCO complexes undergo spin transition at the orbitals of metal sites upon illumination, leading to a change in the spin state [53,54,55,56,57,58,59,60,61,62,63,64]. However, assembling SCO units with coordination bonds to form photoresponsive compounds remains highly challenging because minor changes in the coordination environment of metal sites may influence the spin transition to some extent. Through the rational design of molecular structures based on the SCO unit, it is desired to achieve multifunctional molecular materials with controllable photomagnetic properties.

2.2. Photoinduced Structural Change in Organic Molecules

Photochromism refers to the reversible transformation of a chemical substance be-tween two or more forms that exhibit distinct absorption to light [65,66]. Photochromic systems can undergo reversible transformations between distinct states with varying properties, making them widely applicable in data storage, sensors, bioimaging, and nanomachines [67,68,69,70,71,72,73,74,75].
Typical photochromic ligands, for example, are shown in Figure 2. Upon light illumination, the structural changes most commonly observed are trans-to-cis isomerization and ring-opening/ring-closing transitions [75,76,77]. Under ultraviolet light, azobenzene can undergo trans-to-cis isomerization, and the cis isomer can be reverted to the trans form through exposure to visible light or heat [76,77]. For diarylethene, a [2 + 2] photocycloaddition can occur when the distance between parallelly arranged alkene bonds is appropriate [78,79,80,81,82]. Similarly, 9-anthrylmethylphosphonic acid can undergo a [4 + 4] cycloaddition under ultraviolet light when the spatial requirements are satisfied [83,84]. Upon ultraviolet irradiation, dithienylethene can transform from a colorless open-ring state to a colored closed-ring state and can be switched back to its original state via visible light irradiation [85,86]. In the case of spiropyran, ultraviolet irradiation can result in the photochemical cleavage of the C–O bond, resulting in its conversion from the colorless spiropyran state to the colored merocyanine state. Upon turning off the ultraviolet light, it can revert to its initial colorless state [87,88]. Fulgides can transform from a colorless open-ring state to a colored closed-ring state under ultraviolet light and revert to the initial state through a ring-opening reaction when exposed to visible light [89,90].

2.3. Photogenerated Organic Radicals

In addition to photochromic ligands, another important category of photoresponsive ligands is photogenerated organic radicals. These compounds have been used for various applications, such as smart windows, erasable and inkless printing, catalysis, sensing, artificial photosynthesis, and solar cells [91,92,93,94,95].
As shown in Figure 3, pyridine derivatives, viologens, triazoles, 9-anthracene carboxylic acids, and naphthalenediimides can be converted to radicals upon light illumination through electronic transition [96,97,98]. In recent years, there has been a growing interest in the study of not only molecular nanomagnets but also multifunctional metal–organic frameworks with photogenerated radicals [99,100,101].

3. Photomagnetic Properties of Transition Metal Molecular Nanomagnets

The photomagnetic properties of transition metal molecular nanomagnets primarily arise from the alteration of their electronic structures and/or spin states. Light-induced spin state changes could serve as the fundamental mechanism behind photomagnetic properties. For example, in the six-coordination Fe(II) complexes, the transition from a low-spin state to a high-spin state could be induced by light illumination, thereby influencing the magnetic properties of the complexes. The SCO units have been assembled with cyanide to form chains, wherein the spin state, anisotropy, and magnetic interaction were photoswitched to tune the magnetic properties [15,31,32,33,34,102,103]. Additionally, transition metal molecular nanomagnets with photoinduced metal-to-metal electron transfer (MMET) and photoinduced structural changes in the ligands were also reported [104,105]. Reliable experimental characterization is required for understanding the photoinduced mechanism, which is typically accomplished through advanced characterization techniques. The superconducting quantum interference device (SQUID), physical property measurement system (PPMS), and pulsed electron paramagnetic resonance (EPR) spectrometer are commonly employed to determine the photomagnetic properties of molecular nanomagnets [106,107,108,109].

3.1. Photomagnetic Properties of SCO-Type Transition Metal Molecular Nanomagnets

In 2013, Long’s group reported an iron(II) molecular nanomagnet with photomagnetic properties, [Fe(1-propyltetrazole)6](BF4)2 (Figure 4a) [31]. Under an external magnetic field, this complex exhibited fully reversible switching between the S = 0 and S = 2 states. After irradiation by a 505 nm light for 7 h at 10 K, an LIESST effect was observed. The high-spin state showed no significant decay after the light was turned off. An alternating current (AC) magnetic susceptibility measurement was performed using a SQUID magnetometer, which revealed slow magnetic relaxation behavior in the high-spin Fe(II) state under an external magnetic field (Hdc = 2000 Oe) in the temperature range of 1.9–5.0 K, with an effective barrier of 22 K. An analysis of EPR spectra demonstrated that the anisotropy parameters of the light-induced phase of [Fe(1-propyltetrazole)6](BF4)2 agree with the SMM behavior, with a total spin reversal barrier of 72 K. The effective barrier of 22 K from ac magnetic susceptibility is lower than that of the total spin reversal barrier due to the presence of vibronic coupling, typically observed in mononuclear SMMs. In the same year, Smith’s group reported another iron(II) molecular nanomagnet with photomagnetic properties, PhB(MesIm)3FeII-N = PPh3 (Figure 4b). After 18 h of white light irradiation at 10 K, an LIESST effect was observed. Magnetic susceptibility measurements under light irradiation indicated a transition from the low-spin state to the high-spin state. The high-spin complex exhibited slow magnetic relaxation behavior under an external magnetic field (Hdc = 1000 Oe) in the temperature range of 1.8–4.6 K, with an effective barrier of 22 K [32].
Cyanide-bridged SCO complexes have shown intriguing photoinduced magnetic properties. These complexes generally consist of divalent or trivalent iron/cobalt ions linked by cyanide ligands, resulting in either chain or three-dimensional framework structures. From 2013 onwards, Liu’s group reported a series of molecular nanomagnets with photomagnetic properties, including {[FeIII(Tp*)(CN)3]2FeII(bpmh)}·2H2O, (bpmh, N,N′-bis-pyridin-4ylmethylene hydrazine), {[FeIII(bpy)(CN)4]2[CoII(phpy)2]}·2H2O, (bpy, 2,2′-bipyridine, phpy, 4-phenylpyridine), {[W(CN)8][(FeII)(bib)2](bibH)}·2CH3OH, {[(pzTp)FeIII(CN)3]4FeII2(Pmat)4}n·12H2O, {[pzTpFeII(CN)3]4CoII2(Bib)4}·3H2O, and {[pzTpFeII(CN)3]2CoII(Bpi)2}·CH3CN·4H2O [15,33,34,102,103] (Figure 4c–g). {[FeIII(Tp*)(CN)3]2FeII(bpmh)}·2H2O is a double zigzag chain that includes Fe(II) spin-crossover units and well-isolated paramagnetic Fe(III) ions. This chain exhibited thermally reversible SCO at the Fe(II) sites. Following 12 h of irradiation with 473 nm blue light at 5 K, an SCM behavior was triggered, accompanied by the LIESST effect at the Fe(II) sites and synergistic ferromagnetic coupling between the photoinduced high-spin Fe(II) and low-spin Fe(III) ions [33] (Figure 5).
In 2021, Liu’s group reported a molecular nanomagnet with photomagnetic properties in the form of {[W(CN)8][(FeII)(bib)2](bibH)}·2CH3OH, which exhibited a reversible LIESST effect when subjected to alternating infrared (808 nm) and blue (473 nm) light, enabling reversible switching between paramagnetic high-spin and diamagnetic low-spin states of the Fe(II) center [15]. At 1.8 K, irradiation with infrared light generated SCM behavior due to the magnetic interactions between the photogenerated high-spin Fe(II) centers and tungsten(V) centers, accompanied by wide magnetic hysteresis loops and a large coercive field of 19 kOe (Figure 6a). Irradiation by blue light resulted in isolated Fe(II)–W(V) species exhibiting SMM behavior. Magnetic hysteresis loops measured at 3.3 K showed that the high-spin Fe(II) state under infrared light maintained a relatively narrow hysteresis loop, while the low-spin Fe(II) state under blue light led to the closure of the hysteresis loop (Figure 6b). This represents an interesting example of reversible switching between SCM and SMM accompanied by light-controlled magnetic hysteresis loop switching.

3.2. Photomagnetic Properties of Other Transition Metal Molecular Nanomagnets

Dithienylethene is a photochromic molecule that undergoes reversible ring-opening and ring-closing reactions when exposed to light of different wavelengths, resulting in significant alterations to its electronic and optical properties. In 2009, Irie’s group reported a chain-like molecular nanomagnet based on closed-ring dithienylethene, [Mn4(hmp)6(dae-c)2(H2O)2](ClO4)2·CH3CN·4H2O (Mn4-c; Hhmp = 2-hydroxymethylpyridine, H2dae = 1,2-bis(5-carboxyl-2-methyl-3-thienyl)perfluorocyclopentene) [104]. Upon irradiation with visible light (λ > 480 nm), the closed-ring Mn4-c underwent an open-ring reaction, which enhanced the magnetic interactions between the [Mn4] units and altered its slow magnetic relaxation behavior. In 2019, Yamashita’s group reported zero-dimensional molecular nanomagnets with open-ring and closed-ring dithienylethene, [Mn2(saltmen)2(dae-o)] (Mn2-o) and [Mn(saltmen)(dae-c)]·H2O·Et3N (Mn-c) (H2saltmen = 2,2′-((1E,1′E)-((2,3-dimethylbutane-2,3-diyl)bis(azaneylylidene))bis(methaneylylidene))diphenol, H2dae = 1,2-bis(5-carboxyl-2-methyl-3-thienyl)perfluorocyclopentene) [105]. Under an external magnetic field, the photoproducts Mn2-o-UV and Mn-c-vis exhibited a change in AC magnetic susceptibilities compared to Mn2-o and Mn-c. The effective energy barriers were 15.89, 18.10, 13.96, and 19.91 K for Mn2-o, Mn2-o-UV, Mn-c, and Mn-c-vis, respectively.
Cyano-bridged heterometallic {FeCo} chain systems provide the opportunity to achieve photoswitchable SCMs via light-induced MMET [110,111]. A cyanide-bridged chain {[(Tp)Fe(CN)3]2Co(BIT)}·2CH3OH (Tp = hydrotris(pyrazolyl)borate, BIT = 3,4-bis-(1H-imidazol-1-yl)thiophene) exhibits reversible, multi-phase transitions driven by MMET [110]. Light-irradiated single-crystal X-ray diffraction reveals that MMET occurs exclusively between the Co center and one Fe site, switching the chain between diamagnetic [(Fe1)ᴵᴵLS–CoᴵᴵᴵLS–(Fe2)ᴵᴵᴵLS] and metastable ferromagnetic [(Fe1)ᴵᴵᴵLS–CoᴵᴵHS–(Fe2)ᴵᴵᴵLS] properties at low temperatures. At 10 K, alternating 946 and 532 nm illumination enables the reversible on–off switching of SCM behavior. Moreover, rapid thermal quenching traps a distinct supercooled phase (HTsc, P212121), which differs from both the low-temperature phase (LT, Pnma) and the light-induced high-temperature phase (HT*, P21/n). In addition, removal of lattice methanol upon desolvation suppresses MMET and SCM behavior, underscoring the essential role of hydrogen bonding in tuning redox potentials. These findings establish {[(Tp)Fe(CN)3]2Co(BIT)}·2CH3OH as an uncommon platform that integrates light-, thermal-, and solvent-responsive SCM.

4. Photomagnetic Properties of Lanthanide Molecular Nanomagnets

The combination of photoresponsive ligands with lanthanide ions could result in photoresponsive molecular nanomagnets, which have important applications for high-density data storage, quantum information processing, and optical switches. This strategy combines the strong magnetic anisotropy of lanthanide ions with the dynamic characteristics of photoresponsive ligands. In recent years, researchers have assembled lanthanide ions with photocyclization organic compounds and radical precursors as photoresponsive units to construct various lanthanide molecular nanomagnets with photomagnetic properties [27,28,29,30,112,113,114,115,116,117,118,119,120,121,122] (Figure 7 and Table 1).

4.1. Photomagnetic Properties of Photocyclization-Type Lanthanide Molecular Nanomagnets

Photocyclization-type organic ligands include diarylethene, 9-anthrylmethylphosphonic acids, dithienylethenes, spiropyrans, fulgides, and so on [123,124,125,126,127], which have been employed as photoresponsive units in lanthanide molecular nanomagnets. Diarylethenes and 9-anthrylmethylphosphonic ligands can undergo [2 + 2] and [4 + 4] cycloaddition reactions, respectively, under ultraviolet light [27,28,112,113]. Dithienylethene can undergo cycloaddition reaction when exposed to the light of a specific wavelength [29]. It is worth noting that 9-diethylphosphonomethylanthracene (depma) can undergo photoinduced or thermally induced ring-opening reactions, enabling reversible structural conversions [28,113].
To date, the photomagnetic properties of photocyclization-type lanthanide molecular nanomagnets are primarily focused on [2 + 2] and [4 + 4] cycloaddition reactions induced by light based on the alterations of the coordination environment of the metal centers [27,28,112,113].
The photoinduced cyclization process of 1,2-bis(4-pyridyl)ethylene (bpe) primarily occurs through a [2 + 2] cycloaddition reaction. Under illumination, the double bonds of bpe interact with another molecule, leading to the formation of a cyclobutane structure. In 2015, Tong’s group reported a mononuclear Dy(III) complex with bpe, [Dy(bpe)(H2O)4(NO3)2](NO3)·2bpe [27], where the alkene bonds were arranged parallel at a distance of 3.67 Å. Upon UV irradiation, a [2 + 2] cycloaddition reaction occurred, yielding a binuclear Dy(III) complex, [Dy2(tpcb)(H2O)8(NO3)4](NO3)2·2bpe·tpcb (tpcb = tetrakis(4-pyridyl)cyclobutane) (Figure 8a,b). Under a zero-dc field, the mononuclear complex exhibited slow magnetic relaxation, while the photoproduced binuclear complex displayed only a very weak temperature-dependent magnetic relaxation (Figure 8c,d).
In 2017, another mononuclear Dy(III) complex (Hbpe)2[Dy(bpe)(H2O)(4-pyO)(NO3)(SCN)3]SCN with bpe [112] was reported, where the alkene bonds were parallel with a distance of 3.44 Å. UV irradiation induced a [2 + 2] cycloaddition reaction, yielding a binuclear Dy(III) complex (Hbpe)2(H2tpcb)[Dy2(tpcb)2(H2O)2(4-pyO)2(NO3)2(SCN)6](SCN)2 (tpcb = tetrakis(4-pyridyl)cyclobutane, 4-pyO = 4-(1H)-pyridone) (Figure 8e,f). Subtle changes in the coordination environment around the Dy(III) ions increased the effective energy barrier from 153.8 K (Hdc = 0 Oe) and 201.9 K (Hdc = 1500 Oe) in the mononuclear complex to 205.5 K (Hdc = 0 Oe) and 234.5 K (Hdc = 1500 Oe) in the binuclear complex (Figure 8g,h) [128]. However, in the temperature range dominated by the Raman process, the magnetic relaxation time of the binuclear complex under the 1500 Oe field was significantly shorter compared to the mononuclear complex.
Similarly to the [2,2] cycloaddition of bpe, 9-diethylphosphonomethylanthracene (depma) can undergo a [4,4] cycloaddition reaction upon illumination. Under ultraviolet light, the π bonds of two anthracene rings interacted to form a dimer with an eight-membered ring structure. In 2018, Zheng’s group reported a mononuclear Dy(III) complex, DyIII(depma)(NO3)3(hmpa)2 (hmpa = hexamethylphosphoramide) [28], where the anthracene rings were arranged parallel to each other with an interplanar distance of 3.44 Å. UV irradiation at 365 nm induced a [4 + 4] cycloaddition reaction, forming a binuclear DyIII2(depma2)(NO3)6(hmpa)4 (Figure 9a,b). Under a 500 Oe field, the effective energy barriers of 20.4 K for the mononuclear complex and 43.2 K for the binuclear complex were obtained (Figure 9c,d). Exposure to 254 nm of UV irradiation or thermal treatment reverted the binuclear complex to the mononuclear complex, leading to a reduced effective energy barrier of 18.0 K. This light-driven reversibility highlights the wavelength-dependent switching capabilities.
In 2020, another depma-based mononuclear Dy(III) complex, DyIII(SCN)3(depma)2(4-hpy)2 (1; 4-hpy = 4-hydroxypyridine) [113], was reported, where the anthracene rings were arranged parallel to each other with an interplanar distance of 3.49 Å at 300 K (1RT) and 3.52/3.56 Å at 193 K (1LT). UV irradiation at 365 nm induced a [4 + 4] cycloaddition reaction, leading to a one-dimensional Dy(III) complex 1UV. 1UV reverted to 1 upon heating at 120 °C (Figure 9e). The one-dimensional Dy(III) complex had a different dc magnetic susceptibility compared to the mononuclear complex, and heating at 1UV yielded 1R, which exhibited the same DC magnetic susceptibility as 1 (Figure 9f). Under zero field, the effective energy barriers of 1, 1UV, and 1R were 141, 101, and 153 K, respectively (Figure 9g–i). This work demonstrates the feasibility of switching magnetic properties via light and heat.
Dithienylethene is another photoresponsive ligand. The double bond of ethylene could react with two thiophene groups to form a closed-loop structure under ultraviolet irradiation. Upon exposure to visible light or heating, the closed-loop structure can revert to the open-loop structure, which is a reversible process. In 2020, Bernot’s group reported a one-dimensional Dy(III) complex [Dy(Tppy)F(Lc)]PF6 (1c; Tppy = tris(3-(2-pyridyl)pyrazolyl)hydroborate, L = bispyridyl dithienylethene) with a bispyridyl dithienylethene ligand [29]. Upon irradiation using 532 nm green light, the ligand underwent a transformation from a closed-ring to an open-ring structure, resulting in the formation of the open-ring one-dimensional complex 1o (Figure 10a,b). An in-depth study on the multiple relaxation processes of molecular nanomagnets is crucial for clarifying their dominant mechanisms across different temperature ranges. 1o and 1c exhibited Raman, Orbach, and quantum tunneling relaxation processes with the same effective energy barrier of 225.9 K. Here, τ−1 = τQTM−1 + τ0−1exp(−Ueff/kBT) + BTn was used to fit the relaxation data [19]. 1o and 1c showed the Orbach process at a high temperature range and QTM at a low temperature range. However, 1o (τQTM = 0.0015 s) demonstrated a faster quantum tunneling rate compared to 1c (τQTM = 0.0337 s), and exhibited narrower hysteresis loops (Figure 10c,d). Ab initio calculations indicated that the photomodulation of the magnetic properties originated from the change in crystal packing rather than ligand isomerization-induced crystal field splitting.

4.2. Photomagnetic Properties of Photogenerated Radical-Type Lanthanide Molecular Nanomagnets

Compared to photocyclization-type systems, photogenerated radical families usually exhibit faster response and minimal structural changes. For example, pyridyls and 9-anthracene carboxylic acids are used for lanthanide molecular nanomagnets with photogenerated radicals. If a system employs pyridyl derivatives as electron acceptors and hydroxyethylidene diphosphonate (HEDP) as electron donors, light irradiation induces electron transfer between them, resulting in the generation of stable radicals [30,115]. The aromatic structure could stabilize photogenerated radicals as well. These radicals have the capacity to modulate the coordination field strength of metal centers and/or the magnetic interaction between the metal centers and the radicals.
Wang’s group reported a Dy(III) molecular nanomagnet, [Dy3(H-HEDP)3(H2-HEDP)3]·2H3-TPT·H4-HEDP·10H2O (QDU-1; TPT = 2,4,6-tri(4-pyridyl)-1,3,5-triazine) [30] (Figure 11a). At room temperature and under UV light, colorless QDU-1 transformed into blue QDU-1a, simultaneously generating stable radicals, with a sharp EPR signal at g = 2.0004. Heating at 100 °C for 30 min restored QDU-1 to its colorless state (QDU-1b). Before irradiation, QDU-1 was in a paramagnetic state; after irradiation, the stable radicals induced ferromagnetic interactions with Dy(III) ions at low temperatures, and QDU-1a exhibited SMM behavior (Figure 11b–d), with an effective energy barrier of 108.1 K. Through heating, QDU-1a can be reverted to its initial state. This study represents the observation of room-temperature-reversible photo-thermochromic SMM on/off properties in lanthanide complexes.
In 2021, two photoresponsive lanthanide complexes, [Ln3(H-HEDP)2(H2-HEDP)2(H3-HEDP)2]·H3-TPP·11H2O (Ln = Dy (1-Dy), Tb (2-Tb) and TPP = 2,4,6-tris(4-pyridyl)pyridine) [115], were reported (Figure 11e). At room temperature and under irradiation with a xenon lamp for 40 min, yellow 1-Dy and 2-Tb were transformed to purple 1a-Dy and 2a-Tb with EPR signals at g = 2.014 and 1.996, respectively, from the generation of stable radicals. At low temperatures, antiferromagnetic coupling existed between the lanthanide ions and the photogenerated radicals (Figure 11f). 1-Dy and 2-Tb exhibited SMM behavior, while 1a-Dy and 2a-Tb were paramagnetic (Figure 11g–j). Reversible photo-thermochromic properties and controlled quenching and recovery of SMM behaviors were observed.
The photogenerated crown radicals were proven to be a means to modulate the magnetization of lanthanide complexes. Guo’s group reported a crown-based complex, [DyIII(18C6)(H2O)3]FeIII(CN)6·2H2O (DyFe18C6) [116] (Figure 12a). At room temperature and under UV irradiation, yellow DyFe18C6 transformed into orange DyFe18C6-UV, accompanied by the generation of radicals. Heating at 75 °C for 2 h or storing in darkness for 7 days restored the complex to its initial state. The obtained compound exhibited photochromic and photomagnetic behaviors at room temperature, demonstrating a transition from paramagnetic to ferromagnetic states and a remarkable enhancement of χMT by 20.9% (Figure 12b). DyFe18C6 and its photoproducts had effective energy barriers of 18.4 and 17.0 K, respectively (Figure 12c,d).
Due to the advantages of combining the intrinsic properties of photochromic molecules with those of coordination polymers (CPs)/metal–organic frameworks (MOFs), such as modularity, porosity, and structural adjustability, the application of photoresponsive CPs/MOFs in gas storage and separation has been studied [129,130,131,132,133,134,135]. Since 2013, we have reported a series of SMM-based CPs/MOFs [11,120,121,122,136,137,138,139,140,141,142,143,144,145,146,147,148,149]. However, studies on photoresponsive SMMs in CPs/MOFs remain rare.
In 2023, two Er(III) CPs [Er(CA)1.5(bpy)(DMF)]n (Er(bpy)) and [Er(CA)1.5(phen)(DMF)]n (Er(phen)) (H2CA = 2,5-dichloro-3,6-dihydroxy-p-quinone, bpy = 2,2′-bipyridine, phen = 1,10-phenanthroline) and their light-converted products Er(bpy)-UV and Er(phen)-UV, exhibiting field-induced magnetization dynamics, were reported [120]. The structure of Er(phen) is shown in Figure 13a. The room temperature χMT of Er(phen)-UV increased 25.7% compared with that of Er(phen) (Figure 13b). The EPR signal at g = 2.002 further supported the generation of radicals, influencing the magnetization dynamics. The magnetization dynamics of Er(phen) and Er(phen)-UV were dominated by both Raman and Orbach processes, and Er(phen)-UV showed an enhanced effective energy barrier value compared with that of Er(phen) (Figure 13c,d). It represents an example where both static and dynamic magnetizations of an SMM-based CP were enhanced by UV illumination.
Recently, a SMM-MOF {[Dy1.5(OPh)2Cl(BPy)3(THF)1.5][(BPh4)1.5]·0.5THF}n (Dy(BPy), BPy = 4,4′-bipyridine, OPh− = phenoxide, BPh4− = tetraphenylborate) was reported, which features a pentagonal bipyramid SMM as the node and the photosensitive ligand BPy as the linker [121] (Figure 14a–c). The precise synthesis ensured the equatorial arrangement of BPy and the axial coordination of PhO−, thereby enhancing the vertical orientation of the main magnetic axis of DyIII ions across all Kagomé layers. Dy(BPy) displayed photochromic properties when irradiated with UV light at room temperature, generating radicals, with an EPR signal at g = 2.0000. In comparison to Dy(BPy), Dy(BPy)-UV demonstrates faster relaxation kinetics in the temperature range of 12–70 K and a lower divergence temperature of 6 K in the field cooling and zero-field cooling curves (9 K for Dy(BPy)). The energy barrier of Dy(BPy)-UV was 641 K, which is lower than that of 822 K of Dy(BPy) in the low-temperature domain. The coercivity field sharply decreases from 4500 Oe for Dy(BPy) to 1300 Oe for Dy(BPy)-UV at 2 K, while the hysteresis loop opening temperature diminishes from 20 K for Dy(BPy) to 14 K for Dy(BPy)-UV(Figure 14d,e). A study of the mechanism revealed that the modulated magnetic properties are attributed to the formation of photogenerated radicals and alterations in crystal packing.
9-anthracene carboxylic acid (HACA) serves as a valuable unit for the construction of molecular switches, attributed to its ability to transform into a photogenerated radical. Stable two-dimensional Yb(III) CPs (Yb(ACA)) and their Y(III)-diluted analog Yb@Y(ACA), along with their photogenerated radical forms, Yb(ACA)-UV and Yb@Y(ACA)-UV, were reported [122]. For Yb(ACA) (Figure 15a,b), the formation of the radical leads to an 82.3% enhancement of the static magnetic susceptibilities of Yb(ACA)-UV at room temperature compared to those of Yb(ACA), supported by high-level calculation results, which are among the highest values reported so far (Figure 15c). Unexpected increases in the effective energy barrier for magnetization reversal of Yb(ACA)-UV (111 K) compared with Yb(ACA) (94 K) were observed. This study not only establishes a strategy for designing photomagnetic materials via SMM-based CP platform but also reveals the influence of photogenerated radicals on the static and dynamic magnetizations of lanthanide CPs.

5. Conclusions and Outlook

The recent advances of molecular nanomagnets with photomagnetic properties are summarized. Researchers have applied various strategies to introduce photoresponsive groups into molecular nanomagnets featuring magnetic bistability. Although molecular nanomagnets with photomagnetic properties have received increasing attention in recent years, this field is still in its early stages. Challenges primarily include two aspects: (i) how to rationally synthesize photoresponsive molecular nanomagnets with modulated static and dynamic magnetic properties and (ii) how to achieve reversible switching of the magnetic properties using light. To date, the photomagnetic properties of transition metal molecular nanomagnets are limited mainly to SCO complexes, and the lanthanide molecular nanomagnets are usually connected with photocyclization ligands and photogenerated radicals. Generally, the cycloaddition reaction is restricted by the crystal lattice, leading to slow or even irreversible reactions; photogenerated radicals may not be highly stable, making it challenging to observe the influence of these radicals on magnetic properties quantitatively.
Currently, the static and dynamic magnetic properties of most molecular nanomagnets induced by light decrease in terms of the energy barrier and hysteresis window, and only a limited number of examples demonstrate reversible capability. In addition to the discrete system, CPs and MOFs are a promising platform for the study of molecular nanomagnets with photomagnetic properties, which have the advantages of high stability and the structural flexibility of metal nodes, organic linkers, and guest molecules. Based on the fast development of coordination chemistry and MOF chemistry, research into photoresponsive magnetic CPs and MOFs may develop at a fast pace in the future.

Author Contributions

Conceptualization, W.S., P.C., and X.G.; writing—original draft preparation, X.G.; writing—review and editing, P.C., W.S., X.G., and X.S.; visualization, X.G. and W.S.; funding acquisition, P.C., W.S., and X.G. All authors have read and agreed to the published version of the manuscript.

Funding

This work was supported by the National Natural Science Foundation of China (Grant Nos. 22435002 and 62401563).

Institutional Review Board Statement

Not applicable.

Informed Consent Statement

Not applicable.

Data Availability Statement

No new data were created or analyzed in this study. Data sharing is not applicable to this article.

Conflicts of Interest

The authors declare no conflicts of interest.

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Magnetochemistry 11 00077 g001
Figure 1. Molecular nanomagnets with photomagnetic properties.
Figure 1. Molecular nanomagnets with photomagnetic properties.
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Figure 2. Selected examples of organic molecules with photoinduced structural change groups.
Figure 2. Selected examples of organic molecules with photoinduced structural change groups.
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Figure 3. Selected examples of photoactive organic molecules that can generate stable radicals after illumination.
Figure 3. Selected examples of photoactive organic molecules that can generate stable radicals after illumination.
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Figure 4. Transition metal molecular nanomagnets with photomagnetic properties. (a) [FeII(1-propyltetrazole)6](BF4)2; (b) PhB(MesIm)3FeII-N = PPh3; (c) {[FeIII(Tp*)(CN)3]2FeII(bpmh)}·2H2O; (d) {[FeIII(bpy)(CN)4]2[CoII(phpy)2]}·2H2O; (e) {[W(CN)8][(FeII)(bib)2](bibH)}·2CH3OH; (f) {[(pzTp)FeIII(CN)3]4FeII2(Pmat)4}n·12H2O; (g) {[pzTpFeII(CN)3]4CoII2(Bib)4}·3H2O and {[pzTpFeII(CN)3]2CoII(Bpi)2}·CH3CN·4H2O. Reprinted with permission from Refs. [15,31,32,102] Copyright 2021 Nature Chemistry, 2013 American Chemical Society, 2013 American Chemical Society, and 2021 Angewandte Chemie International Edition. Reprinted from Refs. [33,34,103].
Figure 4. Transition metal molecular nanomagnets with photomagnetic properties. (a) [FeII(1-propyltetrazole)6](BF4)2; (b) PhB(MesIm)3FeII-N = PPh3; (c) {[FeIII(Tp*)(CN)3]2FeII(bpmh)}·2H2O; (d) {[FeIII(bpy)(CN)4]2[CoII(phpy)2]}·2H2O; (e) {[W(CN)8][(FeII)(bib)2](bibH)}·2CH3OH; (f) {[(pzTp)FeIII(CN)3]4FeII2(Pmat)4}n·12H2O; (g) {[pzTpFeII(CN)3]4CoII2(Bib)4}·3H2O and {[pzTpFeII(CN)3]2CoII(Bpi)2}·CH3CN·4H2O. Reprinted with permission from Refs. [15,31,32,102] Copyright 2021 Nature Chemistry, 2013 American Chemical Society, 2013 American Chemical Society, and 2021 Angewandte Chemie International Edition. Reprinted from Refs. [33,34,103].
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Figure 5. The χT–T (a) and χ″–T (b) of {[FeIII(Tp*)(CN)3]2FeII(bpmh)}·2H2O. Reprinted from Ref. [33].
Figure 5. The χT–T (a) and χ″–T (b) of {[FeIII(Tp*)(CN)3]2FeII(bpmh)}·2H2O. Reprinted from Ref. [33].
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Figure 6. Magnetic hysteresis loops of {[W(CN)8][(FeII)(bib)2](bibH)}·2CH3OH at 1.8 K (a) and 3.3 K (b) after irradiation. Reprinted with permission from Ref. [15]. Copyright 2021 Nature Chemistry.
Figure 6. Magnetic hysteresis loops of {[W(CN)8][(FeII)(bib)2](bibH)}·2CH3OH at 1.8 K (a) and 3.3 K (b) after irradiation. Reprinted with permission from Ref. [15]. Copyright 2021 Nature Chemistry.
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Figure 7. Selected examples of lanthanide molecular nanomagnets with photomagnetic properties. Reprinted with permission from Refs. [27,28,29,30,112,113,116,120,121]. Copyright 2015 Chemical Communications, 2018 Angewandte Chemie International Edition, 2019 American Chemical Society, 2020 American Chemical Society, 2017 Inorganic Chemistry Frontiers, 2021 Chemical Science, 2022 Journal of Materials Chemistry C, 2025 Journal of Rare Earths, 2025 American Chemical Society. Reprinted from Ref. [122].
Figure 7. Selected examples of lanthanide molecular nanomagnets with photomagnetic properties. Reprinted with permission from Refs. [27,28,29,30,112,113,116,120,121]. Copyright 2015 Chemical Communications, 2018 Angewandte Chemie International Edition, 2019 American Chemical Society, 2020 American Chemical Society, 2017 Inorganic Chemistry Frontiers, 2021 Chemical Science, 2022 Journal of Materials Chemistry C, 2025 Journal of Rare Earths, 2025 American Chemical Society. Reprinted from Ref. [122].
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Figure 8. The photochemical reaction from [Dy(bpe)(H2O)4(NO3)2](NO3)·2bpe (a) to [Dy2(tpcb)(H2O)8(NO3)4](NO3)2·2bpe·tpcb (b) via [2,2] photocyclization and their frequency-dependent ac susceptibilities (c,d). Reprinted with permission from Ref. [27]. Copyright 2015 Chemical Communications. The photochemical reaction from (Hbpe)2[Dy(bpe)(H2O)(4-pyO)(NO3)(SCN)3]SCN (e) to (Hbpe)2(H2tpcb)[Dy2(tpcb)2(H2O)2(4-pyO)2(NO3)2(SCN)6](SCN)2 (f) via a [2,2] photocyclization and their ln(τ) vs. T−1 plots (g,h). Reprinted with permission from Ref. [112]. Copyright 2017 Inorganic Chemistry Frontiers.
Figure 8. The photochemical reaction from [Dy(bpe)(H2O)4(NO3)2](NO3)·2bpe (a) to [Dy2(tpcb)(H2O)8(NO3)4](NO3)2·2bpe·tpcb (b) via [2,2] photocyclization and their frequency-dependent ac susceptibilities (c,d). Reprinted with permission from Ref. [27]. Copyright 2015 Chemical Communications. The photochemical reaction from (Hbpe)2[Dy(bpe)(H2O)(4-pyO)(NO3)(SCN)3]SCN (e) to (Hbpe)2(H2tpcb)[Dy2(tpcb)2(H2O)2(4-pyO)2(NO3)2(SCN)6](SCN)2 (f) via a [2,2] photocyclization and their ln(τ) vs. T−1 plots (g,h). Reprinted with permission from Ref. [112]. Copyright 2017 Inorganic Chemistry Frontiers.
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Figure 9. The photochemical reaction from DyIII(depma)(NO3)3(hmpa)2 (a) to DyIII2(depma2)(NO3)6(hmpa)4 (b) via [4,4] photocyclization and their ln(τ) vs. T−1 plots (c,d). Reprinted with permission from Ref. [28]. Copyright 2018 Angewandte Chemie International Edition. Structural transformation among 1RT, 1LT, and 1UV (e). The χMT vs. T (f) and ln(τ) vs. T−1 plots (g–i) for 1, 1UV, and 1R. Reprinted with permission from Ref. [113]. Copyright 2021 Chemical Science.
Figure 9. The photochemical reaction from DyIII(depma)(NO3)3(hmpa)2 (a) to DyIII2(depma2)(NO3)6(hmpa)4 (b) via [4,4] photocyclization and their ln(τ) vs. T−1 plots (c,d). Reprinted with permission from Ref. [28]. Copyright 2018 Angewandte Chemie International Edition. Structural transformation among 1RT, 1LT, and 1UV (e). The χMT vs. T (f) and ln(τ) vs. T−1 plots (g–i) for 1, 1UV, and 1R. Reprinted with permission from Ref. [113]. Copyright 2021 Chemical Science.
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Figure 10. The photochemical reaction from 1c (a) to 1o (b) via photocyclization and their τ–T (c) and magnetic hysteresis loops (d). Reprinted with permission from Ref. [29]. Copyright 2019 American Chemical Society.
Figure 10. The photochemical reaction from 1c (a) to 1o (b) via photocyclization and their τ–T (c) and magnetic hysteresis loops (d). Reprinted with permission from Ref. [29]. Copyright 2019 American Chemical Society.
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Figure 11. The structure of QDU-1 (a). The χMT–T (b) and ac susceptibilities (c,d) of QDU-1, QDU-1a, and QDU-1b. Reprinted with permission from Ref. [30]. Copyright 2020 American Chemical Society. The structure of 1-Ln (e). The χMT–T (f) and ac susceptibilities (g–j) of 1-Dy, 1a-Dy, 2-Tb, and 2a-Tb. Reprinted with permission from Ref. [115]. Copyright 2022 Science China Materials.
Figure 11. The structure of QDU-1 (a). The χMT–T (b) and ac susceptibilities (c,d) of QDU-1, QDU-1a, and QDU-1b. Reprinted with permission from Ref. [30]. Copyright 2020 American Chemical Society. The structure of 1-Ln (e). The χMT–T (f) and ac susceptibilities (g–j) of 1-Dy, 1a-Dy, 2-Tb, and 2a-Tb. Reprinted with permission from Ref. [115]. Copyright 2022 Science China Materials.
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Figure 12. Crystal structure of DyFe18C6 (a). The χMT–T (b) and ac susceptibilities (c,d) of DyFe18C6 and DyFe18C6-UV. Reprinted with permission from Ref. [116]. Copyright 2022 Journal of Materials Chemistry C.
Figure 12. Crystal structure of DyFe18C6 (a). The χMT–T (b) and ac susceptibilities (c,d) of DyFe18C6 and DyFe18C6-UV. Reprinted with permission from Ref. [116]. Copyright 2022 Journal of Materials Chemistry C.
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Figure 13. The structure of Er(phen) (a). The χMT–T (b) and ln(τ)–T−1 plots (c,d) for Er(phen) and Er(phen)-UV. Reprinted with permission from Ref. [120]. Copyright 2025 Journal of Rare Earths.
Figure 13. The structure of Er(phen) (a). The χMT–T (b) and ln(τ)–T−1 plots (c,d) for Er(phen) and Er(phen)-UV. Reprinted with permission from Ref. [120]. Copyright 2025 Journal of Rare Earths.
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Figure 14. Structure of [Dy(OPh)X(BPy)4(THF)]+ (X = Cl/PhO−) cation in Dy(BPy) viewed from the side (a) and from above (b). Kagomé layer of Dy(BPy) (c). The magnetic hysteresis loops of Dy(BPy) (d) and Dy(BPy)-UV (e). Reprinted with permission from Ref. [121]. Copyright 2025 American Chemical Society.
Figure 14. Structure of [Dy(OPh)X(BPy)4(THF)]+ (X = Cl/PhO−) cation in Dy(BPy) viewed from the side (a) and from above (b). Kagomé layer of Dy(BPy) (c). The magnetic hysteresis loops of Dy(BPy) (d) and Dy(BPy)-UV (e). Reprinted with permission from Ref. [121]. Copyright 2025 American Chemical Society.
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Figure 15. The photochemical reaction from Yb(ACA) to Yb(ACA)-UV (a). EPR spectra of Yb(ACA) and Yb(ACA)-UV (b). The χMT–T (c) and ln(τ)–T−1 plots (d,e) of Yb(ACA) and Yb(ACA)-UV. Reprinted from Ref. [122].
Figure 15. The photochemical reaction from Yb(ACA) to Yb(ACA)-UV (a). EPR spectra of Yb(ACA) and Yb(ACA)-UV (b). The χMT–T (c) and ln(τ)–T−1 plots (d,e) of Yb(ACA) and Yb(ACA)-UV. Reprinted from Ref. [122].
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Table 1. The static and dynamic magnetic properties of selected photoresponsive lanthanide molecular nanomagnets discussed in this review.
Table 1. The static and dynamic magnetic properties of selected photoresponsive lanthanide molecular nanomagnets discussed in this review.
Complex/
Photoproduct		Photochemical
Reaction 		χMT
at RT
cm3 mol−1 K		Hysteresis
Loop at 2 K
Hc (Oe)		Ueff (K)
Hdc (Oe)		Ref.
[Dy(bpe)(H2O)4(NO3)2](NO3)·2bpe[2,2] cycloaddition13.9--
(slow magnetization relaxation)		[27]
[Dy2(tpcb)(H2O)8(NO3)4](NO3)2·2bpe·tpcb14.2--
(Hbpe)2[Dy(bpe)(H2O)(4-pyO)(NO3)(SCN)3]SCN with bpe[2,2] cycloaddition13.9-
(butterfly-shaped)		153.8 (Hdc = 0)
201.9 (Hdc = 1500)		[112]
(Hbpe)2(H2tpcb)[Dy2(tpcb)2(H2O)2(4-pyO)2(NO3)2(SCN)6](SCN)213.9-
(smaller butterfly-shaped)		205.5 (Hdc = 0)
234.5 (Hdc = 1500)
DyIII(depma)(NO3)3(hmpa)2[4 + 4] cycloaddition13.8-20.4 (Hdc = 500)[28]
DyIII2(depma2)(NO3)6(hmpa)414.1-43.2 (Hdc = 500)
DyIII(SCN)3(depma)2(4-hpy)2 (1)[4 + 4] cycloaddition14.1-
(butterfly-shaped)		141 (Hdc = 0)[113]
1UV14.0-101 (Hdc = 0)
1R14.1-
(butterfly-shaped)		153 (Hdc = 0)
[Dy(Tppy)F(Lc)]PF6 (1c)ring opening13.9-
(butterfly-shaped)		225.9 (Hdc = 0)[29]
1o13.8-
(smaller butterfly-shaped)		225.9 (Hdc = 0)
[Dy3(H-HEDP)3(H2-HEDP)3]·2H3-TPT·H4-HEDP·10H2O (QDU-1)photogenerated radical42.7--(SMM off)[30]
QDU-1a43.7-108.1 (Hdc = 0)
QDU-1b42.7--(SMM off)
[Ln3(H-HEDP)2(H2-HEDP)2(H3-HEDP)2]·H3-TPP·11H2O (Ln = Dy (1-Dy))photogenerated radical42.6-16.9 (Hdc = 2000)[115]
1a-Dy41.8--(SMM off)
[Ln3(H-HEDP)2(H2-HEDP)2(H3-HEDP)2]·H3-TPP·11H2O (Ln = Tb (2-Tb))35.2-12.1 (Hdc = 2000)
2a-Tb33.3--(SMM off)
[DyIII(18C6)(H2O)3]FeIII(CN)6·2H2O (DyFe18C6)photogenerated radical14.5-18.4 (Hdc = 800)[116]
DyFe18C6-UV17.1-17.0 (Hdc = 800)
[Er(CA)1.5(phen)(DMF)]n (Er(phen))photogenerated radical11.5-66.4 (Hdc = 600)[120]
Er(phen)-UV14.4-72.7 (Hdc = 600)
{[Dy1.5(OPh)2Cl(BPy)3(THF)1.5][(BPh4)1.5]·0.5THF}n ((Dy(BPy))photogenerated radical20.57Hc = 4500 Oe822 (Hdc = 0, T = 12–40 K)
1048 (Hdc = 0, T = 53–71 K)		[121]
Dy(BPy)-UV20.63Hc = 1300 Oe641 (Hdc = 0, T = 12–40 K)
1000 (Hdc = 0, T = 53–71 K)
[Yb(CA)(ACA)(DMF)(H2O)]n (Yb(ACA))photogenerated radical2.65-94 (Hdc = 800)[122]
Yb@Y(ACA)-UV4.83-111 (Hdc = 800)
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Gou, X.; Sun, X.; Cheng, P.; Shi, W. Molecular Nanomagnets with Photomagnetic Properties: Design Strategies and Recent Advances. Magnetochemistry 2025, 11, 77. https://doi.org/10.3390/magnetochemistry11090077

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Gou X, Sun X, Cheng P, Shi W. Molecular Nanomagnets with Photomagnetic Properties: Design Strategies and Recent Advances. Magnetochemistry. 2025; 11(9):77. https://doi.org/10.3390/magnetochemistry11090077

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Gou, Xiaoshuang, Xinyu Sun, Peng Cheng, and Wei Shi. 2025. "Molecular Nanomagnets with Photomagnetic Properties: Design Strategies and Recent Advances" Magnetochemistry 11, no. 9: 77. https://doi.org/10.3390/magnetochemistry11090077

APA Style

Gou, X., Sun, X., Cheng, P., & Shi, W. (2025). Molecular Nanomagnets with Photomagnetic Properties: Design Strategies and Recent Advances. Magnetochemistry, 11(9), 77. https://doi.org/10.3390/magnetochemistry11090077

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