arXiv subjects

Thuc T. Mai

Publications and source records attributed to Thuc T. Mai.

At least 19 recordsLinked to original sources

arXiv2026

Towards the First Realization of Weyl Magnons in the Non-Coplanar Antiferromagnet MnTe$_2$

Using a combination of band representation analysis, inelastic neutron scattering (INS), magneto-Raman spectroscopy measurements, and linear spin wave theory, we establish that the non-coplanar antiferromagnet MnTe$_2$ is a tunable Weyl magnon material, hosting symmetry-protected topological nodal lines in its magnon band structure, protected by the the non-coplanar nature of the antiferromagnetic ordering, that transition into Weyl magnons upon the application of symmetry-breaking perturbations using an external magnetic field. By constructing a spin model that reproduces the observed INS magnon spectra and field-dependence of the Raman $Γ$-magnons, we directly probe the topological magnon nodal lines and observe their associated signature of non-trivial topology through the pseudo-spin winding of the scattering intensity in angular scans near the nodal lines. Finally, we discuss the emergence of Weyl magnons in the spectrum through an external magnetic field, and analyze the associated magnon thermal Hall effect allowed by the cubic-symmetry breaking and the associated magnon surface modes, shedding light on future in-field INS and thermal Hall experiments. This work establishes a clear magnonic analog to Weyl electrons, enabling further exploration of topological behavior in bosonic systems and highlighting the interplay between magnetic order and band topology in non-coplanar antiferromagnets.

cond-mat.mtrl-sci↗

arXiv2026

Measuring chiral phonons

Chiral phonons are quantized vibrations where the atomic motion in a solid breaks improper rotation symmetries. In many cases, chiral phonons possess angular momenta and are therefore selective to circularly polarized light. Both fundamental and applied research efforts on chiral phonons have been gaining increasing attention owing to their importance in a variety of fields including spintronics, spin-selective chemical reactions, thermal transport, quantum information processing and biosensing, where the bi-directional spin-lattice coupling enabled by chiral phonons can be harnessed in new ways, and potentially lead to new functionalities. Thus far, the studies of chiral phonons across diverse materials platforms have evolved largely independently within these fields, but the experimental techniques are often interrelated. In this perspective, we present a detailed description, as well as advantages and disadvantages of the current approaches for experimentally measuring chiral phonons in chiral and achiral materials. We conclude with a discussion of new methods for measuring chiral phonons. Ultimately, this work seeks to offer an experimental guide for systematically investigating the properties of chiral phonons in various materials systems and applications.

cond-mat.mtrl-sci↗

arXiv2026

Transport Enhancement and In Situ Control of Electronic Correlation via Photoinduced Modulation Doping of van der Waals Heterostructures

Modulation doping, a well-established technique for traditional semiconductor heterostructures, is a promising approach for tailoring carrier concentration in 2D materials devices. In this letter we report on photoinduced modulation doping in hBN-graphene-hBN-SiO2 heterostructures utilizing standard white light sources and no additional fabrication complexity. We establish the use of this technique to both dope the channel material and to photoanneal devices, providing control over electronic doping and disorder in the graphene channel. We analyze the transport properties by employing Drude and Landauer transport models, highlighting the ability to reversibly tune the mobility and mean scattering length of the graphene with a high degree of accuracy. This tunability allows us to switch our device between the diffusive and quasi-ballistic transport regimes in situ. We utilize the exceptional control our technique provides over local disorder to realize quantum Hall isospin ferromagnetic states in a device whose initial quality would otherwise leave such states unobservable. These results demonstrate precise manipulation of carrier density and charge disorder in van der Waals heterostructures, providing a highly accessible approach to creating high-quality devices capable of realizing correlated electronic states.

cond-mat.mes-hall↗

arXiv2026

Ultraviolet Exciton-Polaritons in Silver Phenylthiolate

Ultraviolet (UV) exciton-polaritons (EPs) enable nonlinear optics, polaritonic lasing, and polariton-mediated photochemistry in the short-wavelength regime, yet progress has been limited due to the scarcity of materials that combine large oscillator strength with stable and narrow UV excitons. Here, we demonstrate UV EPs in silver phenylthiolate (Thiorene, AgSPh), a van der Waals (vdW) layered metal-organic chalcogenolate (MOC) that forms a natural multi-quantum-well (MQW) architecture showing strong excitonic features. Imaging spectroscopic ellipsometry reveals a pronounced in-plane excitonic resonance at 3.46 eV with a narrow linewidth of ~ 60 meV, strong UV birefringence (Δn ~ 0.3), and a high refractive index (n ~ 2.1). Temperature-dependent photoluminescence (PL) shows excitonic emission with a large Stokes shift and substantial exciton-phonon coupling. In both open (self-cavity) and closed cavities, thickness-dependent and angle-resolved reflectance spectra exhibit clear anticrossing, yielding large Rabi splittings of approximately 500 meV. These values are among the largest reported in the UV, positioning thiorene as a promising platform for UV polariton lasers and polariton-enabled photochemistry.

physics.optics↗

arXiv2026

Raman and Terahertz Spectroscopy of Low-Frequency Chiral Phonons in Amino Acids

Chiral phonons are mirror-symmetric vibrations that correspond to twisting and rotational motions of atoms. In chiral biomolecules, they correspond to low-energy terahertz (THz)-range vibrations of the molecular segments involving dozens of atoms whose energies are sensitive to the chirality of the molecules and local atomic geometries. Here we present spectral signatures of chiral phonons in circularly polarized low-frequency Raman and Raman optical activity (ROA) spectra from crystals of several amino acids in different enantiomeric forms. Along with complementary THz circular dichroism (TCD) measurements, our ROA data reveal two sets of bisignate peaks in valine, alanine, tyrosine and proline between 1 and 4.5 THz that are more intense than the ROA peaks in the fingerprint region. Density functional theory (DFT) calculations on L-alanine attribute these modes to twisting and shearing molecular motions. The strong agreement between the ROA and TCD data demonstrates the power of these complementary vibrational spectroscopy techniques to identify chiral phonons in biomolecules, and offers new insights into their vibrational properties and interactions with circularly polarized light.

cond-mat.mtrl-sci↗

arXiv2025

Accurate Angle-Resolved Raman Spectroscopy Methodology: Quantifying the Dichroic Edge Filter Effect

Angle-resolved Raman spectroscopy (ARRS) is an effective method to analyze the symmetry of phonons and other excitations in molecules and solid-state crystals. While there are several configurations of ARRS instruments, the measurement system detailed here utilizes two pairs of linear polarizers and superachromatic half-wave plates. After the orientations of the linear polarizers are set to fixed angles, the two half-wave plates rotate independently, through motorized control, enabling 2D linear polarization mapping. Described within is a protocol to achieve high quality ARRS measurements leveraging phonons from easily accessible test materials [molybdenum disulfide (MoS_2), sapphire (Al_2O_3) and silicon] to validate the system and operation. Quantitative polarized Raman data strongly depends on the quality of sample surface and the optics: the order of placement, alignment, and any distortion caused by their coatings. This study identifies the impact of commonly used edge filters on the polarization response of materials with an anisotropic response as emulated by the T_2g phonon in the Si(100). We detect and model the significant distortion of the T_2g phonon polarization response originating from our dichroic edge filters, the results of which are broadly applicable to optics in any Raman instrument. This ARRS setup also enables helicity-resolved Raman measurements by replacing the first half-wave plate with a superachromatic quarter-wave plate; this configuration is also validated using the Raman response of the aforementioned test materials. This paper aims to increase the quality and reproducibility of polarized Raman measurements through both instrumental considerations and methodology.

physics.optics↗

arXiv2025

Strong Raman Optical Activity and Chiral Phonons in Chiral Hybrid Organic-Inorganic Perovskites

Hybrid organic-inorganic perovskites with chiral organic cations are very interesting for optoelectronic applications because of their intrinsically chiral light-matter interactions. Chiral distortions in these materials lead to circular dichroism, circular birefringence, and circularly polarized luminescence in the band transitions of the inorganic sublattice. Raman-active vibrational modes in these crystals are governed by crystal symmetry and therefore are also strongly impacted by the nature and magnitude of the chiral distortions. Here, we report low-frequency Raman modes that are sensitive to circularly polarized excitation in chiral hybrid organic-inorganic perovskites (CHOIPs) across a wide range of structures and compositions. The circularly polarized Raman spectra from enantiomers of CHOIP single crystals exhibit sharp modes below 150 cm-1, corresponding to vibrations of the lead iodide octahedra. These modes exhibit strong differences in intensities (Raman optical activity, ROA) depending on the handedness of the excitation, with high degree of polarization for several modes. Calculations reveal the presence of several chiral phonon modes with opposite phonon angular momenta. The strong ROA and the chiral phonon modes are a direct consequence of chirality transfer from the chiral organic linker to the lead iodide octahedra in the CHOIP structure, resulting in a strong chiroptical response in the phonon modes.

cond-mat.mtrl-sci↗

arXiv2025

Spin-lattice entanglement in $\mathbf{CoPS}_3$

Complex chalcogenides in the $M$PS$_3$ family of materials ($M$ = Mn, Fe, Co, and Ni) display remarkably different phase progressions depending upon the metal center orbital filling, character of the P-P linkage, and size of the van der Waals gap. There is also a stacking pattern and spin state difference between the lighter and heavier transition metal-containing systems that places CoPS$_3$ at the nexus of these activities. Despite these unique properties, this compound is under-explored. Here, we bring together Raman scattering spectroscopy and infrared absorption spectroscopy with X-ray techniques to identify a structural component to the 119 K magnetic ordering transition as well as a remarkable lower temperature set of magnon-phonon pairs that engage in avoided crossings along with a magnetic scattering continuum that correlates with phonon lifetime effects. These findings point to strong spin-phonon entanglement as well as opportunities to control these effects under external stimuli.

cond-mat.str-el↗

arXiv2025

Anomalous Raman scattering in layered AgCrP$_2$Se$_6$: Helical modes and excitation energy-dependent intensities

Structural anisotropy in layered two-dimensional materials can lead to highly anisotropic optical absorption which, in turn, can profoundly a^ect their phonon modes. These e^ects include lattice orientation-dependent and excitation energy-dependent mode intensities that can enable new phononic and optoelectronic applications. Here, we report anomalous Raman spectra in single-crystalline AgCrP$_2$Se$_6$, a layered antiferromagnetic material. Density functional theory calculations and experimental measurements reveal several unique features in the Raman spectra of bulk and exfoliated AgCrP$_2$Se$_6$ crystals including three helical vibrational modes. These modes exhibit large Raman optical activities (circular intensity di^erences) in bulk AgCrP$_2$Se$_6$, which progressively decrease with thickness. We also observe strong excitation energy dependent peak intensities as well as a decrease in anti-Stokes peak intensities at room temperature with increasing excitation energy, resulting in an apparent cooling by up to 220 K. All of these anomalies in bulk and exfoliated flakes are attributed to the unique ABC layer stacking structure of AgCrP$_2$Se$_6$ and to the smaller unit cell volume that causes hybridization between the Se and Ag/Cr electron densities, resulting in charge transfer and strongly a^ecting the electron-phonon coupling. This work thus positions AgCrP$_2$Se$_6$ as an exciting new 2D material for optical and phononic applications.

cond-mat.mes-hall↗

arXiv2024

Spin-Orbital-Lattice Coupling and the Phonon Zeeman Effect in the Dirac Honeycomb Magnet CoTiO$_3$

The entanglement of electronic spin and orbital degrees of freedom is often the precursor to emergent behaviors in condensed matter systems. With considerable spin-orbit coupling strength, the cobalt atom on a honeycomb lattice offers a platform that can make accessible the study of novel magnetic ground states. Using temperature-dependent Raman spectroscopy and high-magnetic field Raman and infrared (IR) spectroscopy, we studied the lattice and spin-orbital excitations in CoTiO$_3$, an antiferromagnetic material that exhibits topologically protected magnon Dirac crossings in the Brillouin zone. Under the application of an external magnetic field up to 22 T along the crystal's $c$-axis, we observed the splitting of both the spin-orbital excitations and a phonon nearby in energy. Using density functional theory (DFT), we identify a number of new modes that below the antiferromagnetic (AFM) transition become Raman-active due to the zone-folding of the Brillouin zone caused by the doubling of the magnetic unit cell. We use a model that includes both the spin and orbital degrees of freedom of the Co$^{2+}$ ions to explain the spin-orbital excitation energies and their behavior in an applied field. Our experimental observations along with several deviations from the model behavior point to significant coupling between the spin-orbital and the lattice excitations.

cond-mat.str-el↗

arXiv2024

Giant and Tunable Bosonic Quantum Interference Induced by Two-Dimensional Metals

Harnessing quantum interference among bosons provides significant opportunities as bosons often carry longer coherence time than fermions. As an example of quantum interference, Fano resonance involving phonons or photons describes the coupling between discrete and continuous states, signified by an asymmetric spectral lineshape. Utilizing photon-based Fano resonance, molecule sensing with ultra-high sensitivity and ultrafast optical switching has been realized. However, phonon-based Fano resonance, which would expand the application space to a vaster regime, has been less exploited because of the weak coupling between discrete phonons with continuous states such as electronic continuum. In this work, we report the discovery of giant phonon-based Fano resonance in a graphene/2D Ag/SiC heterostructure. The Fano asymmetry, being proportional to the coupling strength, exceeds prior reports by two orders of magnitude. This Fano asymmetry arises from simultaneous frequency and lifetime matching between discrete and continuous phonons of SiC. The introduction of 2D Ag layers restructures SiC at the interface and facilitates resonant scattering to further enhance the Fano asymmetry, which is not achievable with conventional Ag thin films. With these unique properties, we demonstrated that the phonon-based Fano resonance can be used for ultrasensitive molecule detection at the single-molecule level. Our work highlights strong Fano resonance in the phononic system, opening avenues for engineering quantum interference based on bosons. Further, our findings provide opportunities for advancing phonon-related applications, including biochemical sensing, quantum transduction, and superconductor-based quantum computing.

cond-mat.mtrl-sci↗

arXiv2024

Quantum Hall Transport Measurements of Lateral p-n Junctions Formed via Precise Spatial Photodoping of Graphene/hBN Heterostructures

Doped semiconductors are a central and crucial component of all integrated circuits. By using a combination of white light and a focused laser beam, and exploiting hBN defect states, heterostructures of hBN/Graphene/hBN are photodoped in-operando, reproducibly and reversibly. We demonstrate device geometries with spatially-defined doping type and magnitude. After each optical doping procedure, magnetotransport measurements including quantum Hall measurements are performed to characterize the device performance. In the unipolar (p+-p-p+ and n-n+-n) configurations, we observe quantization of the longitudinal resistance, proving well-defined doped regions and interfaces that are further analyzed by Landauer-Buttiker modeling. Our unique measurements and modeling of these optically doped devices reveal a complete separation of the p- and n-Landau level edge states. The non-interaction of the edge states results in an observed "insulating" state in devices with a bi-polar p-n-p configuration that is uncommon and has not been measured previously in graphene devices. This insulating state could be utilized in high-performance graphene electrical switches. These quantitative magnetotransport measurements confirm that these doping techniques can be applied to any 2D materials encapsulated within hBN layers, enabling versatile, rewritable circuit elements for future computing and memory applications.

cond-mat.mes-hall↗

arXiv2024

Ring-Exchange Interaction Effects on Magnons in Dirac Magnet CoTiO$_3$

The magnetic interactions that determine magnetic order and magnon energies typically involve only two spins. While rare, multi-spin interactions can also appear in quantum magnets and be the driving force in the ground state selection and in the nature of its excitations. By performing time-domain terahertz and magneto-Raman spectroscopy measurements combined with theoretical modeling, we determine the origin of the magnon excitation gap in Dirac antiferromagnet CoTiO$_3$. By adding a ring-exchange interaction in a hexagonal plaquette of the honeycomb lattice to both an XXZ spin model and to a low energy spin-orbital flavor wave model, a gap is generated in the magnon spectrum at the Brillouin zone center. With this addition, the flavor wave model reproduces a large swath of experimental results including terahertz, Raman, inelastic neutron scattering, and magnetization experiments.

cond-mat.str-el↗

arXiv2024

Spectroscopy of photoionization from the $^1E$ singlet state in nitrogen$-$vacancy centers in diamond

The $^1E-^1A_1$ singlet manifold of the negatively charged nitrogen vacancy $(NV^-)$ center in diamond plays a central role in the quantum information and quantum sensing applications of the $NV^-$ center. However, the energy of this manifold within the diamond bandgap and with respect to the $^3A_2-^3E$ triplet manifold has not been measured directly. Using field-quenching effects on photoluminescence (PL) spectra, we report on the energy gap between the $^1E-^1A_1$ singlet manifold and the $^3A_2$ and $^3E$ ground and excited triplet states of the $NV^-$ as a function of excitation wavelength and power, temperature, and applied magnetic field in a heavily nitrogen-doped sample. Increased PL and decreased zero-phonon line width from the $NV^0$ were observed in the presence of an applied magnetic field, indicating ionization from the long-lived $^1E$ singlet state. A temperature-dependent ionization threshold between 532 nm and 550 nm was found, locating the singlet states within the diamond band gap.

quant-ph↗

arXiv2023

Raman fingerprints of spin-phonon coupling and magnetic transition in an organic molecule intercalated Cr2Ge2Te6

The manipulation of spin-phonon coupling in both formations and explorations of magnetism in two-dimensional van der Waals ferromagnetic semiconductors facilitates unprecedented prospects for spintronics devices. The interlayer engineering tunes spin-phonon coupling significantly and holds the promise for controllable magnetism via organic cation intercalation. Here, we present spectroscopic evidence to reveal the intercalation effect on intrinsic magnetic and electronic transitions in quasi-two-dimensional Cr2Ge2Te6 using tetrabutyl ammonium as the intercalant. The temperature-evolution of Raman modes E_g^3 and A_g^1, along with the magnetization measurements, unambiguously captures the enhancement of the ferromagnetic Curie temperature in the intercalated heterostructure. Moreover, the E_g^4 mode highlighted the increased effect of spin-phonon interaction in magnetic order-induced lattice distortion. Combined with the first-principle calculations, we observed a substantial number of electrons transferred from TBA+ to Cr through the interface. These results provide the interplay between spin-phonon coupling and magnetic ordering in van der Waals magnets where Raman fingerprints would be highly beneficial for further understanding the manipulation of magnetism in layered heterostructures.

cond-mat.mtrl-sci↗

arXiv2022

Specifics of the Elemental Excitations in "True One-Dimensional" MoI$_3$ van der Waals Nanowires

We report on the temperature evolution of the polarization-dependent Raman spectrum of exfoliated MoI$_3$, a van der Waals material with a "true one-dimensional" crystal structure that can be exfoliated to individual atomic chains. The temperature evolution of several Raman features reveals anomalous behavior suggesting a phase transition of a magnetic origin. Theoretical considerations indicate that MoI$_3$ is an easy-plane antiferromagnet with alternating spins along the dimerized chains and with inter-chain helical spin ordering. The calculated frequencies of the phonons and magnons are consistent with the interpretation of the experimental Raman data. The obtained results shed light on the specifics of the phononic and magnonic states in MoI$_3$ and provide a strong motivation for future study of this unique material with potential for spintronic device applications.

cond-mat.mes-hall↗

arXiv2022

Room temperature ferromagnetism in intercalated Fe3-xGeTe2 van der Waals magnet

Among several well-known transition metal-based compounds, the van der Waals (vdW) Fe3-xGeTe2 (FGT) magnet is a strong candidate for use in two-dimensional (2D) magnetic devices due to its strong perpendicular magnetic anisotropy, sizeable Curie temperature (TC ~ 154 K), and versatile magnetic character that is retained in the low-dimensional limit. While the TC remains far too low for practical applications, there has been a successful push toward improving it via external driving forces such as pressure, irradiation, and doping. Here we present experimental evidence of a novel room-temperature (RT) ferromagnetic phase induced by the electrochemical intercalation of common tetrabutylammonium cations (TBA+) into FGT bulk crystals. We obtained Curie temperatures as high as 350 K with chemical and physical stability of the intercalated compound. The temperature-dependent Raman measurements in combination with vdW-corrected ab initio calculations suggest that charge transfer (electron doping) upon intercalation could lead to the observation of RT ferromagnetism. This work demonstrates that molecular intercalation is a viable route in realizing high-temperature vdW magnets in an inexpensive and reliable manner.

cond-mat.mtrl-sci↗

arXiv2020

Magnon-phonon hybridization in quasi-2D antiferromagnet MnPSe$_3$

Magnetic excitations in van der Waals (vdW) materials, especially in the two-dimensional (2D) limit, are an exciting research topic from both the fundamental and applied perspectives. Using temperature-dependent, magneto-Raman spectroscopy, we identify the hybridization of two-magnon excitations with two separate E$_\mathrm{g}$ phonons in MnPSe$_3$, a magnetic vdW material that could potentially host 2D antiferromagnetism. Results from first principles calculations of the phonon and magnon spectra further support our identification. The Raman spectra's rich temperature dependence through the magnetic transition displays an avoided-crossing behavior in the phonons' frequency and a concurrent decrease in their lifetimes. We construct a model based on the interaction between a discrete level and a continuum that reproduces these observations. The strong magnon-phonon hybridization reported here highlights the need to understand its effects on spin transport experiments in magnetic vdW materials.

cond-mat.mtrl-sci↗