Orbital currents play a fundamental role in a wide range of transport phenomena. Recently, the discovery of a novel chiral orbital current state in the ferrimagnetic nodal-line semiconductor Mn3Si2Te6 has attracted significant interest, supported by anomalous IV characteristics and time-dependent bistable switching. However, the direct experimental verifications, combining electrical transport and magnetic measurement, that detect the variation of the magnetic properties vs the current are still rare. Here, we investigate the transport properties of Mn3Si2Te6 and track the current-induced dynamics of the magnetic moment. Reflective magnetic circular dichroism reveals that significant alterations in Mn3Si2Te6 magnetoresistance in response to an electric field are necessarily coupled with a magnetic phase transition, establishing a rare correlation. Our findings indicate the predominance of magnetic chiral orbital currents in the colossal angular magnetoresistance effect, offering a unique platform for advanced studies in orbital magnetism.

Orbital currents, which refer to the flow of electrons carrying orbital angular momentum, play a fundamental role in a wide range of transport phenomena, including the spin Hall and valley Hall effects.1,2 Orbital currents have garnered significant attention due to their capacity to enrich the research value of material systems. Initial investigations focused on high-temperature superconducting cuprates,3–10 where the presence of orbital currents is considered a pivotal step in understanding materials that lack inversion symmetry. Subsequent research has extended to other systems, such as iridates11–13 and moiré heterostructures.14–16 Furthermore, Kagome superconductors and magnets are recognized as ideal platforms to investigate the interplay between topology, superconductivity, and electron–electron correlations.17–20 Despite this progress, the study of orbital transport remains in its infancy and lags behind that of spin transport; many fundamental principles and novel transport effects are yet to be discovered.2 Recently, the discovery of a novel chiral orbital current (COC) state in the ferrimagnetic nodal-line semiconductor Mn3Si2Te6 has garnered considerable attention.21 

Initial intrigue is sparked by the observation of an extraordinary Colossal Angular Magnetoresistance (CAMR) effect with unique magnetic properties in Mn3Si2Te6,22–28 characterized by a staggering seven-order-of-magnitude drop in magnetoresistance at a 14 T magnetic field applied along the c-axis. This metal-to-insulator transition is also observed under high-pressure conditions of 2 GPa.29,30 Moreover, the anomalous Nernst effect is observed in Mn3Si2Te6.31 In the previous model, this metal–insulator transition is attributed to nodal-line band degeneracy induced by the c-axis magnetic field, which shifts one of the bands toward the Fermi surface.32 Within this framework, the degeneracy of nodal-line bands under magnetic fields is ascribed to spin polarization. Then, the work by Zhang et al. proposed a new perspective; they thought that spin polarization alone is insufficient to account for the drastic magnetoresistance changes observed in Mn3Si2Te6.21 This is further substantiated by neutron diffraction experiments, which corroborate their notion.33 According to their interpretation, the colossal angular magnetoresistance effect originates from a dramatic alteration in the orbital magnetic moment when exposed to changes in the magnetic field. When the magnetic field is zero, the Te atomic sites with opposite directions of the orbital magnetic moments (MCOC) are randomly distributed, and thus, the summational net orbital moment is close to zero. The direction of MCOC could be further switched by the out-of-plane magnetic field, leading to the rapid increase of the net MCOC. This abrupt change induces strong coupling effects, thereby triggering a rapid surge in conductance within the ab-plane. In such a scenario, it is expected to carry out an experimental verification combining electrical transport and in situ magnetic measurement, which can detect the variation of the magnetic properties vs the current through the sample under a cryogenic and high-magnetic field environment.

In this work, we synthesize high-quality Mn3Si2Te6 single crystals with flat surfaces; its ferrimagnetic magnetism is confirmed by magnetic measurements, and the unique nonlinear current vs voltage (IV) behavior is measured by the electrical transport measurement. Furthermore, based on a low-temperature and high-magnetic transport measurement system, we build a reflective magnetic circular dichroism (RMCD) system, which is used to detect the variation of magnetic property in real time through magneto-optical signals while applying current to the Mn3Si2Te6 sample. We find that when the current applied to the sample reaches a threshold where a sharp rise of resistance occurs in the IV curve, the magneto-optical signal is synchronously attenuated violently. It indicates that the increase of current leads to a phase transition in the system, which results in a sharp increase in resistance and a significant decrease in magnetic moment. This kind of exotic current-induced dynamics of the magnetic property reveals that significant alterations in Mn3Si2Te6 magnetoresistance in response to an electric field are necessarily coupled with a transition of magnetic property, establishing a rare yet crucial correlation. Our results further support the perspective provided by the previous report that the COC state plays important roles in the magnetic and transport properties of Mn3Si2Te6,21 offering a unique platform for advanced studies in orbital magnetism.

The nodal-line semiconductor Mn3Si2Te6 features a quasi-two-dimensional structure with a tripartite crystal symmetry, with the P3̄1c space group (no. 163),22,32,34,35 shown in Figs. 1(a) and 1(b). A robust interlayer antiferromagnetic (AFM) interaction is evident between the localized spins of manganese atoms.22 High-quality single crystals are synthesized via the flux method. Raw materials of Mn (99.95%), Si (99.999%), and Te (99.999%) are mixed in the molar ratio of 1:2:6 in an alumina crucible and sealed within a quartz ampule. The assembly is heated to 1273 K over a 24-h period, maintained at this temperature for an additional 24 h, and then gradually cooled to 973 K over 150 h, where it is held for a further 12 h. Following centrifugation to remove excess Te flux, large Mn3Si2Te6 single crystals are obtained, as shown in Fig. 1(c). Each flake of the sample has a smooth surface in the ab-plane, as shown in Fig. 1(e). In the tests of Laue diffraction and x-ray diffraction (XRD) along the sample surface, one can see the perfect hexagonal diffraction point and (00n) diffraction peaks, respectively, as shown in Figs. 1(d) and 1(e), confirming the c axis perpendicular to the sample surface as well as the high purity of these single crystals. Powder x-ray diffraction (XRD) pattern is presented in Fig. 1(f), with observed peaks aligning well with the P3̄1c space group. The lattice parameters, a = b = 7.05 Å, c = 14.30 Å, are consistent with the earlier reports. Further by energy-dispersive spectroscopy [Fig. 1(g)] equipped on a high-resolution field-emission scanning electron microscope, the respective stoichiometric atomic ratio of Mn:Si:Te = 2.94:2.08:5.96 is verified, conforming the nearly ideal stoichiometry of Mn3Si2Te6.

FIG. 1.

Crystal structure and characterizations. (a) Crystal structure of Mn3Si2Te6. (b) Single layers of the different MnTe6 octahedra. (c) The photograph of the single crystal. (d) The Laue diffraction spots obtained along the [001] direction. (e) Single crystal XRD and (f) power XRD spectrum of Mn3Si2Te6. (g) EDS of the Mn3Si2Te6 sample.

FIG. 1.

Crystal structure and characterizations. (a) Crystal structure of Mn3Si2Te6. (b) Single layers of the different MnTe6 octahedra. (c) The photograph of the single crystal. (d) The Laue diffraction spots obtained along the [001] direction. (e) Single crystal XRD and (f) power XRD spectrum of Mn3Si2Te6. (g) EDS of the Mn3Si2Te6 sample.

Close modal

After the high-quality single crystals of Mn3Si2Te6 are obtained, we measure the magnetic and transport properties of these samples. The magnetization M is measured functions of magnetic field H and temperature T. Figure 2(a) demonstrates the change in magnetic properties during the zero-field-cooling (ZFC) process for both magnetic field directions for H//ab plane (blue line) and H//c axis (red line) under H = 1000 Oe. When cooling the temperatures lower than 80 K, a significant increase in the susceptibility χ can be observed according to both two ZFC curves, indicating a magnetic phase transition near the temperature of 80 K. The susceptibility enhancement for H//ab is much more significant compared with H//c, demonstrating the magnetic anisotropy of the Mn3Si2Te6 crystal. Figure 2(b) displays the M-H curves under various temperatures from T = 10–100 K for the H//ab plane. One can see that the spontaneous magnetization around low magnetic fields drops rapidly when the temperature rises up to 80 K and evolves to a linear MH behavior when the temperature is higher than 100 K, consistent with the magnetic transition temperature around 80 K observed in Fig. 2(a). Figure 2(c) shows the magnetization vs external magnetic field (MH) of the sample at the temperature of 2 K for H//ab plane (blue line) and H//c axis (red line). One can clearly see that the saturation magnetization Ms = 1.5 μB/Mn for the case of H//ab reaches under a relatively low field at 0.1 T. However, the magnetization for H//c slowly increases with the magnetic field and saturates with Ms = 1.5 μB/Mn around 8 T, confirming a ferrimagnetic ordering with the easy axis lay in the ab plane.27,28 In addition, we also carry out the electrical transport measurements of our samples. Figure 2(d) presents the temperature-dependent resistance of Mn3Si2Te6 revealing a cusp feature at a temperature around 80 K, corresponding to the magnetic phase transition observed in magnetic measurements. One can also see that upon cooling to 10 K from 80 K, the resistance increases by four orders of magnitude relative to the one at critical temperature. Furthermore, the magnetoresistance is measured at 10 K, and the results are displayed in the inset in Fig. 2(d). Within a magnetic field up to 5 T, one can see that the magnetoresistance for H//c (red line) experiences a substantial decline by nearly four orders of magnitude, while the one only decreases by 60% for H//ab (blue line), demonstrating a pronounced colossal angular magnetoresistance (CAMR) effect.

FIG. 2.

Magnetic and transport properties. (a) Temperature-dependent magnetic susceptibility χ(T) of Mn3Si2Te6 for H//c (red) and H//ab (blue) at H = 1000 Oe. (b) Magnetization for H//ab under different temperatures. (c) Field-dependent magnetization of Mn3Si2Te6 for H//c (red) and H//ab (red), T = 2 K. (d) Resistivity of Mn3Si2Te6 at various temperatures, inset: magnetic magnetoresistance ρ(H)/ρ0 for H//c (blue) and H//ab (red) measured at 10 K.

FIG. 2.

Magnetic and transport properties. (a) Temperature-dependent magnetic susceptibility χ(T) of Mn3Si2Te6 for H//c (red) and H//ab (blue) at H = 1000 Oe. (b) Magnetization for H//ab under different temperatures. (c) Field-dependent magnetization of Mn3Si2Te6 for H//c (red) and H//ab (red), T = 2 K. (d) Resistivity of Mn3Si2Te6 at various temperatures, inset: magnetic magnetoresistance ρ(H)/ρ0 for H//c (blue) and H//ab (red) measured at 10 K.

Close modal

Previous studies have pointed out that this kind of large CAMR effect is related to the chiral orbital currents in Mn3Si2Te6. The chiral orbital currents would lead to exotic current-magnetism coupling in Mn3Si2Te6, and magnetic properties would exhibit unusual current-dependent behavior.21 Unfortunately, since the experimental verification for COC in Mn3Si2Te6 needs to combine magnetic measurement, electrical measurement, and the conditions of low temperature and strong magnetic field simultaneously, the experimental demonstration of this kind of exotic COC-induced current–magnetism coupling is still rare at present. In order to verify this kind of interesting phenomenon, we used a custom-built reflective magnetic circular dichroism (RMCD) system,36 which is also equipped with electrical transport measurement capability. Specifically, to ensure the simultaneous characterization of the magnetism and unique transport phenomenon, like nonlinear IV curve, the low-temperature transport and polar-RMCD measurements were conducted concomitantly in a closed-cycle cryostat equipped with a magnetic coil that can apply a perpendicular magnetic field up to 9 T. The schematic diagram of the experimental setup is displayed in Fig. 3. Samples with flat surfaces were selected to ensure accurate optical measurements. Four electrodes were carefully made by pressing indium on the sample surface. The normally incident circularly polarized beam with a power of 60 µW was focused on the sample between the central electrodes by an objective with a 0.8 numerical aperture. The polar-RMCD signal is proportional to the out-of-plane magnetization at the illuminated spot on the sample. It is measured as the ratio of the differential reflection between the left and right circularly polarized lights and the total reflection. The RMCD signal was detected while the current applied to the sample was varied.

FIG. 3.

RMCD experimental setup. (a) Schematic optical layout for the RMCD measurements in the polar configuration. Beam with 633 nm excitation from the He–Ne laser is modulated by a mechanical chopper, followed by a photoelastic modulator. A beam splitter is placed behind the PEM to pick up the reflected light. The signal is detected by a Si amplified photodetector, and further fed to two lock-in amplifiers to obtain the RMCD ratios I1/I2, where I1 and I2 are the a.c. signal and the reflected signal in the d.c. limit, respectively. Near-normal condition between incident light and sample in a closed-cycle cryostat is satisfied, as shown in (b).

FIG. 3.

RMCD experimental setup. (a) Schematic optical layout for the RMCD measurements in the polar configuration. Beam with 633 nm excitation from the He–Ne laser is modulated by a mechanical chopper, followed by a photoelastic modulator. A beam splitter is placed behind the PEM to pick up the reflected light. The signal is detected by a Si amplified photodetector, and further fed to two lock-in amplifiers to obtain the RMCD ratios I1/I2, where I1 and I2 are the a.c. signal and the reflected signal in the d.c. limit, respectively. Near-normal condition between incident light and sample in a closed-cycle cryostat is satisfied, as shown in (b).

Close modal

The voltage vs current (IV) curves under magnetic fields (T = 15 K) are displayed in Fig. 4(a). A pronounced nonlinear behavior of the IV curves is displayed. Specifically, under zero magnetic field (black line), the IV curve exhibits two transition points, namely, IC1 and IC2. When increasing current from zero amps, the sample is initially quite insulating, and the measured voltage rapidly rises up to 10.18 V under the applied current of 0.4 mA (IC1 under 0 T); however, when the current applied is larger than the threshold of IC1, the voltage continuously declines and reaches a minimum of 1.08 V under 4.6 mA. Subsequently, when the current reaches 15.4 mA, the voltage rises rapidly up to 2.34 V, which marks the emergence of IC2 under 0 T. As for the case of H//c, the decline of IC1 corresponds to the rise in magnetic field and becomes indiscernible when the field is larger than 4 T. Meanwhile, the value of IC2 exhibits a trend of monotonic increasing along with the increasing magnetic field, as shown in the inset in Fig. 4(a). The violent variations of the IV curves observed at the threshold of IC2 signify a phase transition between the COC state and the trivial state. Specifically, the IV behavior of Mn3Si2Te6 governed by Mcoc, the relatively low voltage measured in the IV curve when the applied current is smaller than IC2, is due to the preserved orbital magnetic moments in Mn3Si2Te6, which are aligned uniformly toward the direction of the external magnetic field, and the scattering path of electrons becomes concise, substantially increasing the conductivity. When the current is larger than IC2, the electric field is strong enough to suppress the COC state, an observable decline in magnetic moment coinciding due to the vanish of macroscopic MCOC as well as the voltage discontinuity due to the reestablishing of the electron scattering in the normal state.21 Furthermore, at the same time as the IV measurement, we explore the current-dependent behavior of RMCD signals under magnetic field, as illustrated in Figs. 4(b)4(e). The green curves obtained at 0, 1, 3, and 5 T demonstrate that the RMCD signal is proportional to magnetization. From Figs. 4(b) and 4(c), one can clearly see that there is no significant change in the RMCD signal at IC1, even though the resistance changes. The unchanged magnetic properties at the threshold current of IC1 are inconsistent with the strong coupling of current and magnetism, suggesting a weak relationship between IC1 and the COC state. The curve obtained at 1, 3, and 5 T suggests minimal alteration in the orbital angular momentum prior to its disruption by current. Distinct from the unchanged magnetic properties at IC1, sharp decreases in the RMCD signals can be clearly identified when the applied current touches the threshold of IC2 value under the corresponding field of 1, 3, and 5 T, as shown in Figs. 4(c)4(e), respectively. Upon overlapping the I-RMCD curves with their corresponding IV curves under different magnetic fields, it becomes evident that the decline in magnetic moment exactly coincides with abrupt voltage transitions. The RMCD signal decreases significantly indicating a decrease in the magnetic moments. This is consistent with the previously reported opinion that currents lead to the disruption of orbital magnetism after the COC state is suppressed. It is worth noting that even though there seems an inflection point in the RMCD data, we do not observe the RMCD signal jump under the field of 0 T as the cases under the external field, even though the signal jump on IV curves still can be identified [Fig. 4(b)]. We believe that this is due to the magnetic domains in the sample without applying an external field. Specifically, the sample does not remain well magnetically ordered over the entire area illuminated by the light spot of RMCD measurement, causing relatively small observed RMCD signals. For electrical transport, though the change in magnetism of the entire sample cannot be detected due to the domain at 0 T, the arrangement of the magnetic moments in each domain is still affected by activation or deactivation the of COC state by current. Thus, the microcosmic scattering mechanism of the electronic transport through the sample would still be sensitive to the condition of COC state. This is the reason why the jumping signal of IV behavior can still be observed at IC2 without applying magnetic field in Fig. 4(b). The RMCD measurements provide information on the magnetic moment of Mn3Si2Te6 under electric field. In particular, signals of simultaneous jumps in voltage and magnetic moment are observed, providing direct evidence of current-driven magnetic phase transition in Mn3Si2Te6, further supporting previously reported ideas regarding the COC state.21 Nevertheless, due to the intrinsic limitations of the RMCD measurement technique, the RMCD signal does not precisely quantify the magnetization of the sample. Given the sample’s small magnetic moment and the resultant weak signal, quantitatively analyzing the magnitude of MCOC remains challenging, and extracting other meaningful information requires further in-depth investigations.

FIG. 4.

Electrical transport and in situ magnetic measurement. (a) IV curves at different magnetic fields (0–7.0 T). The inset displays the IC2 value under different magnetic fields, and the error bar of each point is determined by the width of the voltage jumping at IC2 on the corresponding IV curve. (b)–(e) Double-Y axis graphs portraying the I-RMCD curves (green) at different magnetic fields (0, 1.0, 3.0, 5.0 T) and the corresponding IV curves.

FIG. 4.

Electrical transport and in situ magnetic measurement. (a) IV curves at different magnetic fields (0–7.0 T). The inset displays the IC2 value under different magnetic fields, and the error bar of each point is determined by the width of the voltage jumping at IC2 on the corresponding IV curve. (b)–(e) Double-Y axis graphs portraying the I-RMCD curves (green) at different magnetic fields (0, 1.0, 3.0, 5.0 T) and the corresponding IV curves.

Close modal

In conclusion, we grow high-quality single crystals of Mn3Si2Te6, measure the magnetic and transport properties, and observe the previously reported CAMR effect and nonlinear IV curves. To meet experimental requirements, we develop a reflectance magnetic circular dichroism test platform for simultaneous electrical and magnetic measurements under low-temperature and high-magnetic-field conditions, utilizing magneto-optical signals to monitor real-time variations in magnetic properties during current application. Notably, a sharp drop in the magneto-optical signal near the IC2 point on the IV curve indicates a current-driven magnetic phase transition. This reveals that significant changes in Mn3Si2Te6 magnetoresistance in response to an electric field are necessarily associated with magnetic changes, a rare but important correlation. The sensitivity of the Mn3Si2Te6 resistance to magnetic fields and current not only highlights its potential as a magnetic operational platform but also provides a unique opportunity for investigating orbital magnetization. Our findings enhance the understanding of Mn3Si2Te6 intricate magnetic behavior and pave the way for exploring its applications in magneto-electronic devices and quantum technologies.

The authors gratefully acknowledge financial support from the National Key Research and Development Program of China (Grant No. 2022YFA1402404), the National Natural Science Foundation of China (Grant Nos. 92161201, T2221003, 12104221, 12104220, 12274208, 12025404, 12004174, 91961101, 61822403, 11874203, and 12374043), the Natural Science Foundation of Jiangsu Province (BK20230079), and the Fundamental Research Funds for the Central Universities (Grant Nos. 020414380192 and 020414380212).

The authors have no conflicts to disclose.

Z.Z. and G.L. contributed equally to this paper.

Zhixin Zhang: Data curation (lead); Investigation (lead); Writing – original draft (lead). Gan Liu: Investigation (lead); Writing – original draft (equal). Wuyi Qi: Investigation (supporting). Hangkai Xie: Investigation (supporting). Jingwen Guo: Investigation (supporting). Yu Du: Investigation (supporting). Tianqi Wang: Investigation (supporting). Heng Zhang: Investigation (supporting). Fuwei Zhou: Investigation (supporting). Jiajun Li: Investigation (supporting). Yiying Zhang: Investigation (supporting). Yefan Yu: Investigation (supporting). Fucong Fei: Conceptualization (lead); Data curation (equal); Funding acquisition (equal); Resources (equal); Supervision (lead); Writing – original draft (equal); Writing – review & editing (lead). Xiaoxiang Xi: Funding acquisition (equal); Resources (equal); Supervision (equal); Writing – review & editing (equal). Fengqi Song: Funding acquisition (lead); Resources (lead); Supervision (lead); Writing – review & editing (supporting).

The data that support the findings of this study are available from the corresponding authors upon reasonable request.

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