arXiv subjects

Adi Harchol

Publications and source records attributed to Adi Harchol.

6 recordsLinked to original sources

arXiv2026

Spectrally Programmable Spin-Polarized Photocurrents in WSe$_2$-NiPS$_3$ Magnetic van der Waals Heterostructures

Efficient generation and control of spin-polarized currents in semiconductors remain central challenges for spin-based electronics, particularly due to impedance mismatch and the reliance on magnetic fields or ferromagnetic contacts. Here, we introduce a materials platform for spectrally programmable spin transport based on a van der Waals heterostructure combining the antiferromagnetic semiconductor NiPS$_3$ with WSe$_2$. In a p-n diode architecture, circularly polarized excitation produces pronounced photoconductive resonances with spin polarization reaching 80% near the Neel temperature and persisting at 30% at room temperature. Remarkably, selected spectral bands retain their polarization sign across the magnetic phase transition, evidencing robust, spectrally protected spin-polarized current generation. Polarization-resolved photogalvanic measurements reveal a dominant circular injection-current mechanism, confirming spin-polarized carrier transport. First-principles calculations show that an applied electric field induces interfacial hybridization and spin-layer locking, giving rise to localized symmetry breaking and enhanced optical absorption while preserving global time-reversal symmetry. These results establish spectral tuning of excitation as a new control knob for spin transport, enabling spin-current generation without magnetic fields or polarization switching. Our findings position magnetic van der Waals heterostructures as a versatile platform for opto-spintronic functionality and spectrally programmable spintronic devices.

cond-mat.mtrl-sci↗

arXiv2026

Localized Exciton Emission with Spontaneous Circular Polarization in NiPS3/WSe2 Heterostructures

Two-dimensional (2D) van der Waals (vdW) heterostructures (HSs) provide a versatile platform for tailoring electronic, optical, and magnetic properties via proximity effects at their interfaces. In this work, we explore the optical response of few-layer NiPS3/WSe2 HSs using low-temperature micro-photoluminescence ({\mu}-PL) and magneto-PL spectroscopy. The HSs exhibit multiple sharp excitonic peaks that do not appear in the individual constituent materials, indicating the emergence of localized intralayer WSe2 excitons confined by interface-induced potentials. Notably, these excitons exhibit spontaneous circular polarization even in the absence of an external magnetic field, suggesting a magnetic proximity effect induced by uncompensated spins at the NiPS3 interface. Magneto-PL measurements further reveal nonlinear Zeeman splitting, consistent with the presence of an interfacial exchange field that alters the valley exciton dynamics. Density functional theory (DFT) calculations confirm the intralayer origin of the PL and reveal interfacial hybridization and spin texture modifications, supporting the experimental findings. These results highlight how combining a 2D semiconductor with a layered antiferromagnet enables control over valley polarization and spin degrees of freedom, offering new opportunities for chiral light sources and magnetically tunable optoelectronic devices.

cond-mat.mtrl-sci↗

arXiv2026

Evidence for Many-Body States in NiPS$_3$ Revealed by Angle-Resolved Photoelectron Spectroscopy

We present $\mu$-ARPES spectra of the Mott-insulating van der Waals antiferromagnet NiPS$_3$. Signatures of strong correlations -- such as the onset of atomic or atomic-ligand multiplets and spin-orbit-entangled exciton have been observed in this material by various two-particle spectroscopies, but not previously in photoemission. Our measurements reveal a weakly dispersive feature at the valence-band edge that is absent in DFT+$U$ calculations and remains unchanged across the N\'eel transition. After critically examining and ruling out alternative interpretations, we show that an exact diagonalization of a NiS$_6$ cluster yields low-energy final-state configurations of mixed multiplet $d^7$ and $d^8\underline{L}$ character, whose energy differences are consistent with the observed additional feature. This implies that ARPES directly accesses local Ni-S multiplet physics in NiPS$_3$, revealing a many-body structure beyond mean-field theory. Our results confirm that NiPS$_3$ is an excellent model platform in which strong correlations, reduced dimensionality, and covalent metal-ligand bonding jointly shape both two- and single-particle spectroscopies, underscoring the need for a genuinely quantum many-body description of two-dimensional quantum materials.

cond-mat.str-el↗

arXiv2025

Probing the band structure of the strongly correlated antiferromagnet NiPS3 across its phase transition

NiPS3 is an exfoliable van-der-Waals intralayer antiferromagnet with zigzag-type spin arrangement. It is distinct from other TMPS3 (TM: transition metal) materials by optical excitations into a strongly correlated state that is tied to the magnetic properties. However, the related, fundamental band structure across the antiferromagnetic phase transition has not been probed yet. Here, we use angular-resolved photoelectron spectroscopy with {\mu}m resolution in combination with DFT+U calculations for that purpose. We identify a characteristic band shift across TN. It is attributed to bands of mixed Ni and S character related to the superexchange interaction of Ni 3t2g orbitals. Moreover, we find a structure above the valence band maximum with little angular dispersion that could not be reproduced by the calculations. The discrepancy suggests the influence of many-body interactions beyond the DFT+U approximations in striking contrast to the results on MnPS3 and FePS3, where these calculations were sufficient for an adequate description.

cond-mat.str-el↗

arXiv2024

Change in Magnetic Order in NiPS3 Single Crystals Induced by a Molecular Intercalation

Intercalation is a robust method for tuning the physical properties of a vast number of van der Waals (vdW) materials. However, the prospects of using intercalation to modify magnetism in vdWs systems and the associated mechanisms have not been investigated adequately. In this work, we modulate magnetic order in an XY antiferromagnet NiPS3 single crystals by introducing pyridine molecules into the vdWs gap under different thermal conditions. X-ray diffraction measurements indicated pronounced changes in the lattice parameter beta, while magnetization measurements at in-plane and out-of-plane configurations exposed reversal trends in the crystals Neel temperatures through intercalation-de-intercalation processes. The changes in magnetic ordering were also supported by three-dimensional thermal diffusivity experiments. The preferred orientation of the pyridine dipoles within vdW gaps was deciphered via polarized Raman spectroscopy. The results highlight the relation between the preferential alignment of the intercalants, thermal transport, and crystallographic disorder along with the modulation of anisotropy in the magnetic order. The theoretical concept of double-exchange interaction in NiPS3 was employed to explain the intercalation-induced magnetic ordering. The study uncovers the merit of intercalation as a foundation for spin switches and spin transistors in advanced quantum devices.

cond-mat.mtrl-sci↗

arXiv2024

Tuning Magnetic and Optical Properties in MnxZn1-xPS3 Single Crystals by the Alloying Composition

The exploration of two-dimensional (2D) antiferromagnetic (AFM) materials has shown great promise and interest in tuning the magnetic and electronic properties as well as studying magneto-optical effects. The current work investigates the control of magneto-optical interactions in alloyed MnxZn1-xPS3 lamellar semiconductor single crystals, with the Mn/Zn ratio regulating the coupling strength. Magnetic susceptibility results show a retention of AFM order followed by a decrease in N\'eel temperatures down to ~ 40% Mn concentration, below which a paramagnetic behavior is observed. Absorption measurements reveal an increase in bandgap energy with higher Zn(II) concentration, and the presence of Mn(II) d-d transition below the absorption edge. DFT+U approach qualitatively explained the origin and the position of the experimentally observed mid band-gap states in pure MnPS3, and corresponding peaks visible in the alloyed systems MnxZn1-xPS3. Accordingly, emission at 1.3 eV in all alloyed compounds results from recombination from a 4T1g Mn(II) excited state to a hybrid p-d state at the valence band. Most significant, temperature-dependent photoluminescence (PL) intensity trends demonstrate strong magneto-optical coupling in compositions with x > 0.65. This study underscores the potential of tailored alloy compositions as a means to control magnetic and optical properties in 2D materials, paving the way for advances in spin-based technologies.

cond-mat.mtrl-sci↗