arXiv subjects

Nasim Alem

Publications and source records attributed to Nasim Alem.

At least 19 recordsLinked to original sources

arXiv2026

Impact of Cu-Mn ratio on Structure and Defects in Layered Multiferroic Cu1-xMn1+ySiTe3

Multiferroic materials exhibit the coexistence of magnetic and ferroelectric order, enabling control of magnetism through electric fields and vice versa. These properties make them attractive for spintronic and memory device applications. Recent studies on Cu1-xMn1+ySiTe3 (0.04 \leq x \leq 0.26; 0.03 \leq y \leq 0.15) have revealed strong magnetoelectric coupling, with variations in Mn-to-Cu concentration leading to variations in optical, electronic, and magnetic responses. Despite these findings, the influence of nanoscale structure and defects on the observed properties remains poorly understood. In this study, we investigate the structure and nanoscale defects in Cu-deficient Cu1-xMn1+ySiTe3 (Cu:Mn ratio <1, i.e., with 0.04 \leq x \leq 0.26 and 0.03 \leq y \leq 0.15) and Cu-rich Cu1+xMn1-ySiTe3 (Cu:Mn ratio >1, i.e., with 0.04 \leq x \leq 0.3 and 0.13 \leq y \leq 0.31) crystals using scanning/transmission electron microscopy and single-crystal X-ray diffraction. Cu-deficient crystals exhibit extensive stacking faults correlated with chemical inhomogeneity between Mn and Cu, along with variations in Te stacking. In contrast, Cu-rich crystals show fewer stacking faults but contain other local structural variations, such as needle-shaped precipitates and loop-like features. These distinct local structural features between Cu-rich and Cu-deficient crystals can be correlated to variations in their observed properties. Complementary density functional theory calculations confirm that the Cu-rich structure is more polar than the Cu-deficient structure. Overall, this study provides a comprehensive understanding of how subtle changes in chemistry influence the nanoscale structure, defect distribution, and functional properties in Cu1-xMn1+ySiTe3, offering guidance for designing multiferroic materials with tailored performance.

cond-mat.mtrl-sci↗

arXiv2026

Quantifying the coupling between strain and cation valence in high entropy oxide thin films using electron microscopy

High entropy oxides (HEOs) are a class of materials with vast compositional space and tunable properties, making them attractive for applications in thermoelectrics, magnetism, ionic conduction, and beyond. However, their metastable nature makes the local structure, and consequently their properties, highly sensitive to growth conditions. It is therefore essential to probe the local modulations in atomic, chemical, and electronic structure as a function of growth conditions. Here, advanced S/TEM techniques, including 4D-STEM combined with electron energy loss spectroscopy and energy-dispersive X-ray spectroscopy are used to investigate the effect of substrate temperature on structure and strain at the nanoscale regime in HEO thin films. We quantify how nanoscale strain variations correlate with Co valence and subtle chemical differences in the films with the same nominal composition but different growth temperatures. Our results demonstrate that identical HEO compositions can accommodate distinct strain and defect states in thin film form and highlight how synthesis conditions can be leveraged to manipulate strain and Co valence. These findings establish a framework to tailor functional properties via strain and valence control in high entropy oxide thin films.

cond-mat.mtrl-sci↗

arXiv2026

Defect Control via Cu Enrichment Enhances Multifunctional Properties in the Polar Semiconductor Cu1+xMn1-ySiTe3

Polar materials have recently attracted significant interest due to their rich multifunctional properties. The chalcogenide polar semiconductor Cu1-xMn1+ySiTe3 (Cu-deficient) is an emerging multiferroic system in which electric polarization is coupled to magnetization. However, its macroscopic ferroelectric polarization is strongly suppressed due to the presence of a high density of stacking faults. In this work, we demonstrate that these crystal defects, likely originating from non-stoichiometry, can be substantially reduced by increasing the Cu content. Cu-enriched samples, Cu1+xMn1-ySiTe3, crystallize in a noncentrosymmetric monoclinic structure (space group Pm) as the Cu-deficient counterpart but show a nearly stacking-fault-free phase, which is attributed to the emergence of an interstitial site. Consequently, the Cu-enriched samples show a pronounced enhancement of the second-harmonic generation (SHG) response compared to Cu-deficient compositions. Magnetically, the Cu-enriched crystals retain long-range antiferromagnetic order with a Neel temperature of TN ~ 33 K without a glassy state but manifest a distinct spin-flop transition along the polar b-axis that is absent in the Cu-deficient compositions. Furthermore, the electronic ground state evolves from insulating to doped semiconducting behavior upon Cu enrichment. Together, these results establish this material system as a unique and versatile platform for elucidating the interplay among composition, crystal defects, and multifunctional properties, offering a route to design magnetic polar systems with tunable quantum functionalities.

cond-mat.mtrl-sci↗

arXiv2026

Anomalous Crystallinity and Magnetism in Chemically Disordered Coherent Heterostructures

High-entropy oxide (HEO) thin films uniquely superimpose exceptional chemical disorder with exceptional crystalline quality and coherence - an intersection we term anomalous crystallinity that arises from coupled structural, chemical, and valence degrees of freedom unique to the entropy-stabilized condition. Here, we demonstrate unexpected and predictive control of this state using formulation, epitaxial constraints, and kinetic arrest of metastable macrostates. Specifically, aliovalent cation substitutions, tightly controlled substrate temperatures, and conditions favoring significant adatom kinetic energy, can program the out-of-plane lattice parameter of coherent rock salt HEOs while preserving in-plane epitaxial pinning to MgO. Lattice strains exceeding 5% can be stabilized in multilayer heterostructures using this approach, where 3+ cations compensated by cation vacancies predominate the defect chemistry landscape. We highlight the exemplar (Sc,Mg,Co,Ni,Cu,Zn)O/(Cr,Mg,Co,Ni,Cu,Zn)O (JSc/JCr) system where Sc and Cr substitution into the rock salt structure produces pseudomorphic heterostructures between individual antiferromagnets exhibiting exceptional strain and abrupt interfaces across which the Co valence switches from mostly 2+ to an even 2+/3+ mixture. These unprecedented valence interfaces are accompanied by a 2x exchange bias boost compared to single-layer constituents, that could be attributed to enhanced uncompensated spins in the layers themselves or around the buried JSc/JCr interface. These results establish pseudomorphic valence interfaces with anomalous crystallinity as a source of new magnetic macrostates that host emergent magnetic and spintronic functionality.

cond-mat.mtrl-sci↗

arXiv2026

Successful growth of low carrier density $\alpha$-In$_2$Se$_3$ single crystals using Se-flux in a modified Bridgman furnace

Indium selenide (In$_2$Se$_3$) has garnered significant attention for its intriguing properties and applications in batteries, solar cells, photodetectors and ferroelectric devices. However, the controlled synthesis of single phase $\alpha$-In$_2$Se$_3$ remains challenging owing to its complex phase diagram, presence of multiple polymorphs and the high volatility of selenium that induces non-stoichiometry and unintentional carrier doping. For ferroelectric {\alpha}-In2Se3, minimizing the carrier density is essential because leakage current can obscure polarization switching. Here, we report the growth of $\alpha$-In$_2$Se$_3$ single crystals using a unique approach, the Se-flux assisted modified vertical Bridgman technique combined with liquid encapsulation under high pressure. This approach creates a high-pressure, Se-rich environment that effectively minimizes Se-vaporization. Structural and compositional analysis using X-ray diffraction, transmission electron microscopy and energy-dispersive X-ray spectroscopy confirm the formation of pure $\alpha$-In$_2$Se$_3$ single crystals with 3R stacking. Furthermore, the crystals exhibit remarkably low carrier density of 1.5-3.2 $\times$ 10$^{16}$ cm$^{-3}$ at 300K$-$the lowest reported to date, reflecting a significant suppression of Se-vacancies relative to the conventional Bridgman or melt-grown crystals. Through transport and ARPES measurements on different batches of crystals, we also demonstrate that the amount of Se-flux plays a crucial role in controlling Se-vacancies. Our results thus establish this modified Bridgman method as an effective strategy for synthesizing large $\alpha$-In$_2$Se$_3$ single crystals with reduced intrinsic defects. This technique can be broadly applied to grow other volatile chalcogenides with reduced defects and controlled stoichiometry.

cond-mat.mtrl-sci↗

arXiv2025

Resolving Structural Transitions in Lanthanide High-Entropy Oxides

We report a temperature-composition phase diagram for the chemically disordered and CeO2-LA2O3 high entropy oxides (HEOs), where LA denotes equimolar Y, La, Sm, and Pr, delineating stability regions for bixbyite, disordered fluorite, and intermediate vacancy-ordered fluorite phases. The diagram is constructed from a characterization package applied to bulk ceramics including X-ray diffraction (XRD), transmission electron microscopy (TEM) electron diffraction, Raman spectroscopy, energy-dispersive spectroscopy, X-ray absorption near-edge structure spectroscopy, and ultraviolet-visible spectroscopy, to quantify crystal structure at multiple length-scales, local coordination environments, and electronic structures across the formulation space. This comprehensive measurement suite is critical to identify boundaries between the closely related phases. For example, Raman scattering reveals local structural and defect environments unique to bixbyite local order that persist to ~50% Ce under equilibrium synthesis conditions but are invisible to XRD and TEM. We also report a companion thin film study to demonstrate that quenched kinetic energy from a physical deposition process can metastabilize the high symmetry, and thus high entropy, fluorite phase with only 20% Ce. This is noteworthy because electroneutrality constraints demand an exceptionally vacated oxygen sublattice; we estimate 16.7%, approaching that of delta-Bi2O3. Together, our equilibrium ceramics and far-from-equilibrium thin films show that when synthesis is coupled with rigorously chosen, multi-length-scale characterization, now one can identify the phase stability thermodynamic drivers and simultaneously derive practical guidelines for experimentally realizing targeted phases and structures - and thereby deliberately engineer properties in CeO2-LA2O3 HEOs, whose broad defect chemistries demand such an approach.

cond-mat.mtrl-sci↗

arXiv2025

Chemically-Disordered Transparent Conductive Perovskites with High Crystalline Fidelity

This manuscript presents a working model linking chemical disorder and transport properties in correlated-electron perovskites with high-entropy formulations and a framework to actively design them. We demonstrate this new learning in epitaxial Sr$x$(Ti,Cr,Nb,Mo,W)O$3$ thin films that exhibit exceptional crystalline fidelity despite a diverse chemical formulation where most B-site species are highly misfit with respect to valence and radius. X-ray diffraction, X-ray photoelectron spectroscopy, and transmission electron microscopy confirm a unique combination of chemical disorder and structural perfection in thick epitaxial layers. This combination produces significant electron correlation, low electrical resistivity, and an optical transparency window that surpasses that of constituent end-members, with a flattened frequency- and temperature-dependent response. We address the computational challenges of modeling such systems and investigate short-range ordering using cluster expansion. These results showcase that unusual d-metal combinations access an expanded property design space that is predictable using end-member characteristics -- though unavailable to them -- thus offering performance advances in optical, spintronic, and quantum devices.

cond-mat.mtrl-sci↗

arXiv2024

Local structure maturation in high entropy oxide (Mg,Co,Ni,Cu,Zn)1-x(Cr,Mn)xO thin films

High entropy oxides (HEO)s have garnered much interest due to their available high degree of tunability. Here, we study the local structure of (MgNiCuCoZn)0.167(MnCr)0.083O, a composition based on the parent HEO (MgNiCuCoZn)0.2O.We synthesized a series of thin films via pulsed laser deposition at incremental oxygen partial pressures. X-ray diffraction shows lattice parameter to decrease with increased pO2 pressures until the onset of phase separation. X-ray absorption fine structure shows that specific atomic species in the composition dictate the global structure of the material as Cr, Co, and Mn shift to energetically favorable coordination with increasing pressure. Transmission electron microscopy analysis on a lower-pressure sample exhibits a rock salt structure, but the higher-pressure sample reveals reflections reminiscent of the spinel structure. In all, these findings give a more complete picture on how (MgNiCuCoZn)0.167(MnCr)0.083O forms with varying initial conditions and advances fundamental knowledge of cation behavior in high entropy oxides.

cond-mat.mtrl-sci↗

arXiv2024

Quantum Confined Luminescence in Two dimensions

Achieving localized light emission from monolayer two-dimensional (2D) transition metal dichalcogenides (TMDs) embedded in the matrix of another TMD has been theoretically proposed but not experimentally proven. In this study, we used cathodoluminescence performed in a scanning transmission electron microscope to unambiguously resolve localized light emission from 2D monolayer MoSe2 nanodots of varying sizes embedded in monolayer WSe2 matrix. We observed that the light emission strongly depends on the nanodot size wherein the emission is dominated by MoSe2 excitons in dots larger than 85 nm, and by MoSe2/WSe2 interface excitons below 50 nm. Interestingly, at extremely small dot sizes (< 10 nm), the electron energy levels in the nanodot become quantized, as demonstrated by a striking blue-shift in interface exciton emission, thus inducing quantum confined luminescence. These results establish controllable light emission from spatially confined 2D nanodots, which holds potential to be generalized to other 2D systems towards future nanophotonic applications.

cond-mat.mtrl-sci↗

arXiv2024

Order evolution from a high-entropy matrix: understanding and predicting paths to low temperature equilibrium

Interest in high-entropy inorganic compounds originates from their ability to stabilize cations and anions in local environments that rarely occur at standard temperature and pressure. This leads to new crystalline phases in many-cation formulations with structures and properties that depart from conventional trends. The highest-entropy homogeneous and random solid-solution is a parent structure from which a continuum of lower-entropy offspring can originate by adopting chemical and/or structural order. This report demonstrates how synthesis conditions, thermal history, and elastic and chemical boundary conditions conspire to regulate this process in Mg0.2Co0.2Ni0.2Cu0.2Zn0.2O, during which coherent CuO nano-tweeds and spinel nano-cuboids evolve. We do so by combining structured synthesis routes, atomic-resolution microscopy and spectroscopy, density functional theory, and a phase field modeling framework that accurately predicts the emergent structure and local chemistry. This establishes a framework to appreciate, understand, and predict the macrostate spectrum available to a high-entropy system that is critical to rationalize property engineering opportunities.

cond-mat.mtrl-sci↗

arXiv2023

Colossal nonreciprocal Hall effect and broadband frequency mixing due to a room temperature nonlinear Hall effect

Nonreciprocal (NR) charge transport in quantum materials has attracted enormous interest since it offers an avenue to investigate quantum symmetry related physics and holds many prospective applications such as rectification and photodetection over a wide range of frequencies. The NR transport reported to date occurs along the longitudinal direction with the NR resistance limited to a few percent of the ohmic resistance. Here we report a transverse nonreciprocal transport phenomenon with divergent nonreciprocity - colossal NR Hall effect. This is revealed in direct current (DC) measurements on the microscale Hall devices made of the Pt wires deposited by focused ion beam (FIB) on Si substrates and the Weyl semimetal NbP with FIB-deposited Pt electrodes at 0 magnetic field. When a DC is applied along the x-axis of the devices Ix, it generates a voltage along the y-axis Vy near room temperature, with Vy quadratically scaling with Ix. The transverse resistance, which shows a sign reversal upon switching the current direction, results from a colossal extrinsic nonlinear Hall effect (NLHE) rooted in the disorder scatterings in the Pt wires. While NbP was not found to show NLHE, the NLHE generated in the Pt electrodes can be transmitted to the NbP Hall devices, which yields a surprisingly large nonlinear anomalous Hall effect in NbP with the Hall angle (${Θ_H}$) far exceeding the record value of the anomalous Hall angle of magnetic conductors at room temperature. Furthermore, we find such a strong NLHE can lead to broadband frequency mixing, with the frequency spectrum of the Hall voltage including 2nd-harmonic generation, sum & difference frequency generations, and other multiple wave mixing components. These results not only demonstrate the concept of the NRHE for the first time but also pave the way for exploring NLHE's applications in Thz communication, imaging, and energy harvesting.

cond-mat.mes-hall↗

arXiv2023

Valley Isospin Controlled Fractional Quantum Hall States in Bilayer Graphene

A two-dimensional electron system placed in a magnetic field develops Landau levels, where strong Coulomb interactions lead to the appearance of many-body correlated ground states. Quantum numbers similar to the electron spin enable the understanding and control of complex ground state order and collective excitations. Owing to its spin, valley and orbital degrees of freedom, Bernal-stacked bilayer graphene offers a rich platform to pursue correlated phenomena in two dimensions. In this work, we fabricate dual-gated Bernal-stacked bilayer graphene devices and demonstrate unprecedented fine control over its valley isospin degrees of freedom using a perpendicular electric field. Higher sample quality enables us to probe regimes obscured by disorder in previous studies. We present evidence for a new even-denominator fractional quantum Hall state at filling factor ν = 5/2. The 5/2 state is found to be spontaneously valley polarized in the limit of vanishing valley Zeeman splitting, consistent with a theoretical prediction made regarding the spin polarization of the Moore-Read state. In the vicinity of the even-denominator fractional quantum Hall states, we observe the appearance of the predicted Levin-Halperin daughter states of the Moore-Read Pfaffian wave function at ν= 3/2, 7/2, and -1/2 and of the anti-Pfaffian at ν= 5/2. These observations suggest the breaking of particle-hole symmetry in bilayer graphene. We construct a comprehensive valley polarization phase diagram for the Jain sequence fractional states surrounding filling factor 3/2. These results are well explained by a two-component composite fermion model, further demonstrating the SU(2) nature of the valley isospin in bilayer graphene. Our experiment paves the path for future efforts of manipulating the valley isospin in bilayer graphene to engineer exotic topological orders and quantum information processes.

cond-mat.mes-hall↗

arXiv2023

Exciton Confinement in Two-Dimensional, In-Plane, Quantum Heterostructures

Two-dimensional (2D) semiconductors are promising candidates for optoelectronic application and quantum information processes due to their inherent out-of-plane 2D confinement. In addition, they offer the possibility of achieving low-dimensional in-plane exciton confinement, similar to zero-dimensional quantum dots, with intriguing optical and electronic properties via strain or composition engineering. However, realizing such laterally confined 2D monolayers and systematically controlling size-dependent optical properties remain significant challenges. Here, we report the observation of lateral confinement of excitons in epitaxially grown in-plane MoSe2 quantum dots (~15-60 nm wide) inside a continuous matrix of WSe2 monolayer film via a sequential epitaxial growth process. Various optical spectroscopy techniques reveal the size-dependent exciton confinement in the MoSe2 monolayer quantum dots with exciton blue shift (12-40 meV) at a low temperature as compared to continuous monolayer MoSe2. Finally, single-photon emission was also observed from the smallest dots at 1.6 K. Our study opens the door to compositionally engineered, tunable, in-plane quantum light sources in 2D semiconductors.

cond-mat.mes-hall↗

arXiv2022

Strong Room-Temperature Bulk Nonlinear Hall Effect in a Spin-Valley Locked Dirac Material

Nonlinear Hall effect (NLHE) is a new type of Hall effect with wide application prospects. Practical device applications require strong NLHE at room temperature (RT). However, previously reported NLHEs are all low-temperature phenomena except for the surface NLHE of TaIrTe4. Bulk RT NLHE is highly desired due to its ability to generate large photocurrent. Here, we show the spin-valley locked Dirac state in BaMnSb2 can generate a strong bulk NLHE at RT. In the microscale devices, we observe the typical signature of an intrinsic NLHE, i.e. the transverse Hall voltage quadratically scales with the longitudinal current as the current is applied to the Berry curvature dipole direction. Furthermore, we also demonstrate our nonlinear Hall device's functionality in wireless microwave detection and frequency doubling. These findings broaden the coupled spin and valley physics from 2D systems into a 3D system and lay a foundation for exploring bulk NLHE's applications.

cond-mat.mes-hall↗

arXiv2022

Thermally Induced Structural Evolution and Nanoscale Interfacial Dynamics in Layered Metal Chalcogenides

Layered chalcogenides including Bi2Te3, Sb2Te3, Bi-Sb-Te ternary alloys and heterostructures are known as great thermoelectric, topological insulators and recently highlighted as plasmonic building blocks beyond noble metals. Here, we conduct a joint in situ transmission electron microscopy (in situ TEM) and density functional theory (DFT) calculations to investigate the temperature dependent nanoscale dynamics, interfacial properties and further identifying the role of native defects and edge configurations in anisotropic sublimations of Bi2Te3-Sb2Te3 in-plane heterostructure and Sb2-xBixTe3 alloy. Structural dynamics including edge evolution, formation, expansion, and coalescence of thermally induced polygonal nanopores are reported. The nanopores appear to be initiated by preferential dissociation of chalcogenide species (Te) from the center, heterointerface and edges in the heterostructure and only from the outer edges in the alloy counterpart. This results in a reduced thermal stability and significantly different sublimation pathways of the heterostructure. Furthermore, triangular and quasi hexagonal configurations are observed to be the dominant nanopores configurations in the heterostructure. Additionally, our DFT calculations provide a mechanistic understanding on the role of native defects and edge formation energies, revealing the antisite defects TeBi to be the dominant native defect in a Te-rich condition and playing a key role on the defects assisted sublimation. These findings significantly impact our understanding of controlling the nanoscale sublimation dynamics and can ultimately assist us in designing tunable low-dimensional chalcogenides.

cond-mat.mtrl-sci↗

arXiv2022

Delicate Ferromagnetism in MnBi$_6$Te$_{10}$

Tailoring magnetic orders in topological insulators is critical to the realization of topological quantum phenomena. An outstanding challenge is to find a material where atomic defects lead to tunable magnetic orders while maintaining a nontrivial topology. Here, by combining magnetization measurements, angle-resolved photoemission spectroscopy, and transmission electron microscopy, we reveal disorder-enabled, tunable magnetic ground states in MnBi$_6$Te$_{10}$. In the ferromagnetic phase, an energy gap of 15 meV is resolved at the Dirac point on the MnBi$_2$Te$_4$ termination. In contrast, antiferromagnetic MnBi$_6$Te$_{10}$ exhibits gapless topological surface states on all terminations. Transmission electron microscopy and magnetization measurements reveal substantial Mn vacancies and Mn migration in ferromagnetic MnBi$_6$Te$_{10}$. We provide a conceptual framework where a cooperative interplay of these defects drives a delicate change of overall magnetic ground state energies, and leads to tunable magnetic topological orders. Our work provides a clear pathway for nanoscale defect-engineering towards the realization of topological quantum phases.

cond-mat.mtrl-sci↗

arXiv2022

Alloyed B-(AlxGa1-x)2O3 bulk Czochralski single B-(Al0.1Ga0.9)2O3 and polycrystals B-(Al0.33Ga0.66)2O3, B-(Al0.5Ga0.5)2O3), and property trends

In this work, bulk Czochralski-grown single crystals of 10 mol. % Al2O3 alloyed B-Ga2O3 - monoclinic 10% AGO or B-(Al0.1Ga0.9)2O3 - are obtained, which show +0.20 eV increase in the bandgap compared with unintentionally doped B-Ga2O3. Further, growths of 33% AGO - B-(Al0.33Ga0.67)2O3 - and 50% AGO - B-(Al0.5Ga0.5)2O3 or B-AlGaO3 - produce polycrystalline single-phase monoclinic material (B-AGO). All three compositions are investigated by x-ray diffraction, Raman spectroscopy, optical absorption, and 27Al nuclear magnetic resonance (NMR). By investigating single phase B-AGO over a large range of Al2O3 concentrations (10 - 50 mol. %), broad trends in the lattice parameter, vibrational modes, optical bandgap, and crystallographic site preference are determined. All lattice parameters show a linear trend with Al incorporation. According to NMR, aluminum incorporates on both crystallographic sites of B-Ga2O3, with a slight preference for the octahedral (GaII) site, which becomes more disordered with increasing Al. Single crystals of 10% AGO were also characterized by x-ray rocking curve, transmission electron microscopy, purity (glow discharge mass spectroscopy and x-ray fluorescence), optical transmission (200 nm - 20 um wavelengths), and resistivity. These measurements suggest that electrical compensation by impurity acceptor doping is not the likely explanation for high resistivity, but rather the shift of a hydrogen level from a shallow donor to a deep acceptor due to Al alloying. .. Cont. This article may be downloaded for personal use only. Any other use requires prior permission of the author and AIP Publishing. This article appeared in Journal of Applied Physics 131 155702.

cond-mat.mtrl-sci↗

arXiv2022

Crossover of Ising- to Rashba-Type Superconductivity in Epitaxial Bi2Se3/Monolayer NbSe2 Heterostructures

A topological insulator (TI) interfaced with an s-wave superconductor has been predicted to host an unusual form of superconductivity known as topological superconductivity (TSC). Molecular beam epitaxy (MBE) has been the primary approach in the scalable synthesis of the TI/superconductor heterostructures. Although the growth of epitaxial TI films on s-wave superconductors has been achieved, it remains an outstanding challenge for synthesizing atomically thin TI/superconductor heterostructures, which are critical for engineering the TSC phase. Here, we used MBE to grow Bi2Se3 films with the controlled thickness on monolayer NbSe2 and performed in-situ angle-resolved photoemission spectroscopy and ex-situ magneto-transport measurements on these Bi2Se3/monolayer NbSe2 heterostructures. We found that the emergence of Rashba-type bulk quantum well bands and spin-nondegenerate surface states coincides with a marked suppression of the in-plane upper critical magnetic field of the superconductivity in Bi2Se3/monolayer NbSe2 heterostructures. This is the signature of a crossover from Ising- to Rashba-type superconducting pairings, induced by altering Bi2Se3 film thickness. Our work opens a new route for exploring a robust TSC phase in TI/Ising superconductor heterostructures.

cond-mat.supr-con↗