Xinyan Li
Current Organizations / Institutes
The organizations/institutes from the scholar's latest article
Xinyan Li has a total of 312 co-authors. Here are the top co-authors by number of shared publications:
- Yimo Han
Department of Materials Science and Nanoengineering, Rice University, Houston, USA
15 shared publications - Ramamoorthy Ramesh
Lawrence Berkeley National Laboratory
13 shared publications - Sajid Husain
Department of Materials Science and Engineering, University of California, Berkeley, CA, USA
11 shared publications - Darrell G. Schlom
Department of Materials Science and Engineering Cornell University Ithaca New York USA
7 shared publications Qinghua Zhang
Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing, China
7 shared publicationsAng Gao
Beijing National Center for Electron Microscopy and Laboratory of Advanced Materials, Department of Materials Science and Engineering, Tsinghua University, Beijing, China
6 shared publications
Latest Publications
- Open Access
- 30 October 2026
- Published by American Association for the Advancement of Science (AAAS) in Science Advances
- Vol. 12 (44)
Electric field–controlled spin transport in a topological insulator interfaced with a ferroelectric antiferromagnet
Topological insulators have been explored extensively for spin-charge interconversion via magnetic interfaces, yet the true response of their spin-charge conversion, particularly in the absence of an external magnetic field, remains to be studied. Here, we report electric field control of spin-charge conversion in the topological insulator Bi 2 Te 3 with the antiferromagnetic multiferroic BiFeO 3 , using a nonlocal spin transport device. A systematic thickness dependence of the spin transport across the interface between Bi 2 Te 3 and BiFeO 3 reveals a signature of topological surface-state–dominated spin transport in the bilayer system. The spin-charge conversion remains robust for thicknesses above 10 nanometers but falls rapidly with reducing thickness and vanishes at 5 nanometers. This is consistent with hybridization-induced emergence of a trivial insulating phase, which is supported by the coherency factor estimated from the magnetoconductance of Bi 2 Te 3 . These results establish that spin-momentum–locked surface states dominate interfacial spin transport in the decoupled regime. Beyond presenting efficient spin-charge interconversion at an entirely insulating magnetic interface, this work also highlights sputter-deposited Bi 2 Te 3 as a high-quality and scalable platform for integrating quantum materials onto the devices. The nonlocal spin transport approach presented here provides a simple and unprecedented direct evidence of spin-charge conversion and opens an efficient and practical pathway toward designing energy-efficient spin-based devices.
- 30 October 2026
- Published by American Association for the Advancement of Science (AAAS) in Science Advances
- Vol. 12 (44)
Open AccessElectric field–controlled spin transport in a topological insulator interfaced with a ferroelectric antiferromagnet
Topological insulators have been explored extensively for spin-charge interconversion via magnetic interfaces, yet the true response of their spin-charge conversion, particularly in the absence of an external magnetic field, remains to be studied. Here, we report electric field control of spin-charge conversion in the topological insulator Bi 2 Te 3 with the antiferromagnetic multiferroic BiFeO 3 , using a nonlocal spin transport device. A systematic thickness dependence of the spin transport across the interface between Bi 2 Te 3 and BiFeO 3 reveals a signature of topological surface-state–dominated spin transport in the bilayer system. The spin-charge conversion remains robust for thicknesses above 10 nanometers but falls rapidly with reducing thickness and vanishes at 5 nanometers. This is consistent with hybridization-induced emergence of a trivial insulating phase, which is supported by the coherency factor estimated from the magnetoconductance of Bi 2 Te 3 . These results establish that spin-momentum–locked surface states dominate interfacial spin transport in the decoupled regime. Beyond presenting efficient spin-charge interconversion at an entirely insulating magnetic interface, this work also highlights sputter-deposited Bi 2 Te 3 as a high-quality and scalable platform for integrating quantum materials onto the devices. The nonlocal spin transport approach presented here provides a simple and unprecedented direct evidence of spin-charge conversion and opens an efficient and practical pathway toward designing energy-efficient spin-based devices.
- 28 October 2026
- Published by Springer Nature in Nature Materials
- p. 1-8
Altermagnetic signatures and topological textures in ultrathin multiferroic BiFeO3
Magnetoelectric multiferroics promise low-power switching, non-volatile memory and signal transduction, yet practical deployment requires ultrathin films in which polar and magnetic order often degrade. Uncompensated bound charge drives depolarization in ferroelectrics, whereas off-stoichiometry, reduced anisotropy and charge transfer can produce magnetic dead layers. Here we realize a multiferroic phase of BiFeO3 with no dead layer, revealing signatures of emergent altermagnetism in the ultrathin limit. First-principles calculations, symmetry analysis, atomic-resolution imaging and magnetic imaging show that short-circuit electrostatic boundary conditions and epitaxial strain drive a continuous, thickness-induced phase transition accompanied by multiferroic topological textures. At four unit cells, these boundary conditions stabilize a collinear monoclinic phase with d-wave altermagnetic order, supported by magnetic circular dichroism and spin-resolved photoemission measurements. These results establish a pathway to stabilize unconventional multiferroicity at device-relevant thicknesses, reframing scaling limits for oxide electronics.
- 28 October 2026
- Published by Springer Nature in Nature Materials
- p. 1-8
Altermagnetic signatures and topological textures in ultrathin multiferroic BiFeO3
Magnetoelectric multiferroics promise low-power switching, non-volatile memory and signal transduction, yet practical deployment requires ultrathin films in which polar and magnetic order often degrade. Uncompensated bound charge drives depolarization in ferroelectrics, whereas off-stoichiometry, reduced anisotropy and charge transfer can produce magnetic dead layers. Here we realize a multiferroic phase of BiFeO3 with no dead layer, revealing signatures of emergent altermagnetism in the ultrathin limit. First-principles calculations, symmetry analysis, atomic-resolution imaging and magnetic imaging show that short-circuit electrostatic boundary conditions and epitaxial strain drive a continuous, thickness-induced phase transition accompanied by multiferroic topological textures. At four unit cells, these boundary conditions stabilize a collinear monoclinic phase with d-wave altermagnetic order, supported by magnetic circular dichroism and spin-resolved photoemission measurements. These results establish a pathway to stabilize unconventional multiferroicity at device-relevant thicknesses, reframing scaling limits for oxide electronics.
- 5 August 2026
- Published by Springer Nature in Nature
- Vol. 656 (8127) , 349-356
Encapsulation epitaxy of air-stable 2D superconductors for quantum circuits
- 5 August 2026
- Published by Springer Nature in Nature
- Vol. 656 (8127) , 349-356
Encapsulation epitaxy of air-stable 2D superconductors for quantum circuits
- 29 July 2026
- Published by Springer Nature in Nature
- Vol. 656 (8126) , 67-72
Perpendicular switching of polarization in layered ferroelectrics
Ferroelectric materials exhibit a spontaneous electric polarization that can be reversed by an electric field1, a property central to non-volatile memories2,3, sensors4 and actuators5,6. In most conventional ferroelectrics, the polarization originates from a softening of a polar mode7. The amplitude of the mode along a given direction couples with the applied field along the same direction8. Ferroelectrics with a predominant in-plane polarization are harder to use in standard device geometries and therefore the field has mostly focused on out-of-plane ferroelectrics. Developing approaches that enable manipulation of the in-plane polarization component with an out-of-plane field would therefore provide new opportunities for device design and functionality. Here we have discovered that a trilinear coupling between the in-plane and out-of-plane polarization, mediated by means of the octahedral tilts and rotations in the layered ferroelectric Bi4Ti3O12, naturally fulfils this challenge and enables perpendicular switching of the polarization state. In its bulk monoclinic phase, this material hosts a large in-plane polarization (about 50 μC cm-2) driven by a proper ferroelectric instability, together with smaller out-of-plane polarization (about 5 μC cm-2) of improper origin, induced by oxygen octahedral distortions. We demonstrate that, in c-axis-oriented epitaxial films, the in-plane polarization switches deterministically under an out-of-plane electric field. This cross-coupling between orthogonal polarization components provides a route to transverse manipulation of ferroic order parameters and establishes layered ferroelectrics as a platform for capacitive computing concepts.
- 29 July 2026
- Published by Springer Nature in Nature
- Vol. 656 (8126) , 67-72
Perpendicular switching of polarization in layered ferroelectrics
Ferroelectric materials exhibit a spontaneous electric polarization that can be reversed by an electric field1, a property central to non-volatile memories2,3, sensors4 and actuators5,6. In most conventional ferroelectrics, the polarization originates from a softening of a polar mode7. The amplitude of the mode along a given direction couples with the applied field along the same direction8. Ferroelectrics with a predominant in-plane polarization are harder to use in standard device geometries and therefore the field has mostly focused on out-of-plane ferroelectrics. Developing approaches that enable manipulation of the in-plane polarization component with an out-of-plane field would therefore provide new opportunities for device design and functionality. Here we have discovered that a trilinear coupling between the in-plane and out-of-plane polarization, mediated by means of the octahedral tilts and rotations in the layered ferroelectric Bi4Ti3O12, naturally fulfils this challenge and enables perpendicular switching of the polarization state. In its bulk monoclinic phase, this material hosts a large in-plane polarization (about 50 μC cm-2) driven by a proper ferroelectric instability, together with smaller out-of-plane polarization (about 5 μC cm-2) of improper origin, induced by oxygen octahedral distortions. We demonstrate that, in c-axis-oriented epitaxial films, the in-plane polarization switches deterministically under an out-of-plane electric field. This cross-coupling between orthogonal polarization components provides a route to transverse manipulation of ferroic order parameters and establishes layered ferroelectrics as a platform for capacitive computing concepts.
- Open Access
- 29 July 2026
- Published by Springer Nature in Research Square
Hidden liquid-crystalline order in a non-collinear antiferromagnet
Liquid crystals (LCs) provide a canonical framework to understand intermediate phases between liquids and crystals, such as nematic and smectic order, and the rich phenomenology that emerges when such orders are subjected to boundaries, confinement, and elastic frustration. Here, we reveal a hidden mesoscale liquid-crystal-like organization of spin cycloids in a room-temperature magnetoelectric antiferromagnet BiFeO3. It is observed that ferroelectric domain walls act as anchoring surfaces, locally selecting cycloid propagation vectors analogous to surface induced alignment in LCs. Interestingly, confinement imposed by multiple domain walls stabilizes coherent smectic-like cycloidal order in between domain walls through “order by confinement”, while geometrical frustration at domain boundaries induces non-local Helfrich-Hurault–type elastic instabilities in cycloid smectics. Building on these insights, we show that surface-energy engineering dramatically enhances the long range orientational coherence of spin cycloids, enabling robust non-local magnon transport in the ultra-thin limit. These findings establish self-organization as a guiding principle for engineering novel magnetic textures and emergent spin functionalities, opening new opportunities for spintronic and magnonic technologies.
- 29 July 2026
- Published by Springer Nature in Research Square
Open AccessHidden liquid-crystalline order in a non-collinear antiferromagnet
Liquid crystals (LCs) provide a canonical framework to understand intermediate phases between liquids and crystals, such as nematic and smectic order, and the rich phenomenology that emerges when such orders are subjected to boundaries, confinement, and elastic frustration. Here, we reveal a hidden mesoscale liquid-crystal-like organization of spin cycloids in a room-temperature magnetoelectric antiferromagnet BiFeO3. It is observed that ferroelectric domain walls act as anchoring surfaces, locally selecting cycloid propagation vectors analogous to surface induced alignment in LCs. Interestingly, confinement imposed by multiple domain walls stabilizes coherent smectic-like cycloidal order in between domain walls through “order by confinement”, while geometrical frustration at domain boundaries induces non-local Helfrich-Hurault–type elastic instabilities in cycloid smectics. Building on these insights, we show that surface-energy engineering dramatically enhances the long range orientational coherence of spin cycloids, enabling robust non-local magnon transport in the ultra-thin limit. These findings establish self-organization as a guiding principle for engineering novel magnetic textures and emergent spin functionalities, opening new opportunities for spintronic and magnonic technologies.
- Open Access
- 24 July 2026
- Published by Wiley in Advanced Functional Materials
- Vol. 36 (81) , e76779
Optical Signature of Moiré Superlattices Formed by Twisted SrTiO 3 Membranes
Moiré superlattices formed at the interfaces of mismatched lattices have attracted significant interest over the past decade due to their large tunability of band parameters and interactions among electrons, spins, and lattices. Superlattices made from twisted perovskite oxides may have strong structure and potential modulation, but evidence of such modulation over macroscopic areas, particularly at large twisting angles, has not been clearly demonstrated so far. Here, millimeter‐scale twisted oxide bilayers are fabricated at angle, close to the simple coincidence site lattice condition , from freestanding SrTiO 3 membranes. We observe new low‐frequency vibrational modes whose Raman activity, according to molecular dynamics simulations, is greatly enhanced by an asymmetric, twisted interface between the SrO and TiO 2 layers. Such an interface is energetically favorable from first‐principles calculations and is corroborated by the observation of strong second‐harmonic generation from the interface, whose amplitude is comparable to that from the bare SrTiO 3 surface throughout the bilayer region. The results are consistent with interlayer coupling, which is enhanced by high‐temperature annealing and confirmed by cross‐sectional scanning transmission electron microscopy. Our work sheds light on the structural behavior of twisted oxides and provides directions for tuning their phononic and nonlinear optical properties in future studies.
- 24 July 2026
- Published by Wiley in Advanced Functional Materials
- Vol. 36 (81) , e76779
Open AccessOptical Signature of Moiré Superlattices Formed by Twisted SrTiO 3 Membranes
Moiré superlattices formed at the interfaces of mismatched lattices have attracted significant interest over the past decade due to their large tunability of band parameters and interactions among electrons, spins, and lattices. Superlattices made from twisted perovskite oxides may have strong structure and potential modulation, but evidence of such modulation over macroscopic areas, particularly at large twisting angles, has not been clearly demonstrated so far. Here, millimeter‐scale twisted oxide bilayers are fabricated at angle, close to the simple coincidence site lattice condition , from freestanding SrTiO 3 membranes. We observe new low‐frequency vibrational modes whose Raman activity, according to molecular dynamics simulations, is greatly enhanced by an asymmetric, twisted interface between the SrO and TiO 2 layers. Such an interface is energetically favorable from first‐principles calculations and is corroborated by the observation of strong second‐harmonic generation from the interface, whose amplitude is comparable to that from the bare SrTiO 3 surface throughout the bilayer region. The results are consistent with interlayer coupling, which is enhanced by high‐temperature annealing and confirmed by cross‐sectional scanning transmission electron microscopy. Our work sheds light on the structural behavior of twisted oxides and provides directions for tuning their phononic and nonlinear optical properties in future studies.
- Open Access
- 24 July 2026
- Published by American Association for the Advancement of Science (AAAS) in Science Advances
- Vol. 12 (30)
Van der Waals template–encoded soft epitaxy of tellurium enabled by atomic layer deposition
Van der Waals (vdW) epitaxy can integrate lattice-mismatched crystals with atomically sharp, pristine interfaces. However, translating this concept to atomic layer deposition (ALD), a standard for low-temperature, layer-by-layer growth, remains challenging because precursors adsorb transiently on chemically inert vdW basal planes, leading to physisorption-limited nucleation and poor crystalline ordering. Here, we introduce diffusion-steered epitaxial ALD (Epi-ALD), redefining vdW surfaces as programmable kinetic-thermodynamic landscapes and demonstrate highly crystalline tellurium at 150°C. Epi-ALD couples surface-potential-encoded physisorption with long-range diffusion to promote ordered nucleation and epitaxial alignment. This “soft” pathway enables strain-free tellurium epitaxy with a pristine vdW gap (∼1.4 angstrom) despite lattice mismatch (>3.6%) and generalizes across multiple vdW templates. Retaining hallmark advantages of ALD including scalability and uniformity, we further program in-plane orientation through vdW symmetry engineering to achieve quasi-single-crystalline tellurium films with pronounced anisotropy and a chiral anomaly signature. Our work establishes a universal, low-thermal-budget approach for integrating vdW materials and expands the scope of epitaxy within the ALD paradigm.
- 24 July 2026
- Published by American Association for the Advancement of Science (AAAS) in Science Advances
- Vol. 12 (30)
Open AccessVan der Waals template–encoded soft epitaxy of tellurium enabled by atomic layer deposition
Van der Waals (vdW) epitaxy can integrate lattice-mismatched crystals with atomically sharp, pristine interfaces. However, translating this concept to atomic layer deposition (ALD), a standard for low-temperature, layer-by-layer growth, remains challenging because precursors adsorb transiently on chemically inert vdW basal planes, leading to physisorption-limited nucleation and poor crystalline ordering. Here, we introduce diffusion-steered epitaxial ALD (Epi-ALD), redefining vdW surfaces as programmable kinetic-thermodynamic landscapes and demonstrate highly crystalline tellurium at 150°C. Epi-ALD couples surface-potential-encoded physisorption with long-range diffusion to promote ordered nucleation and epitaxial alignment. This “soft” pathway enables strain-free tellurium epitaxy with a pristine vdW gap (∼1.4 angstrom) despite lattice mismatch (>3.6%) and generalizes across multiple vdW templates. Retaining hallmark advantages of ALD including scalability and uniformity, we further program in-plane orientation through vdW symmetry engineering to achieve quasi-single-crystalline tellurium films with pronounced anisotropy and a chiral anomaly signature. Our work establishes a universal, low-thermal-budget approach for integrating vdW materials and expands the scope of epitaxy within the ALD paradigm.
- Open Access
- 10 July 2026
- Published by American Association for the Advancement of Science (AAAS) in Science Advances
- Vol. 12 (28) , eaeh2106
Mechanical control of polar order
BiFeO 3 is a model multiferroic in which the ferroelectric polarization is coupled to ferroelastic lattice distortions, yet deterministic control of its domain structure remains limited by high switching fields and competing polarization variants. Here, we identify a mechanically assisted polarization switching pathway in epitaxial BiFeO 3 thin films that fundamentally alters the switching energetics. Using just out-of-plane electric fields, polarization reversal requires voltages of approximately 4 volts and stabilizes coexisting polarization states. In contrast, when mechanical pressure is applied concurrently, the positive coercive voltage can be substantially reduced, even to 0 volts, resulting in spontaneous switching. Piezoresponse force microscopy measurements reveal that applied mechanical pressure suppresses ferroelastic domain competition, indicating a decrease in the required electrical energy barrier associated with polarization rotation and domain wall motion. This frames the strain field from the AFM tip directly as an effective voltage that assists in ferroelectric switching. By directly coupling lattice distortions to polarization reversal, mechanically assisted switching provides a general framework for controlling coupled order parameters in multiferroic oxides, which can be directly applied in the device-level architecture, where a small mechanical pressure can help in achieving a lower switching energy of ferroelectric polarization. This work advances the fundamental understanding of electromechanical coupling in complex ferroics and establishes mechanical energy as a powerful tool for probing and manipulating ferroelastic-ferroelectric interactions.
- 10 July 2026
- Published by American Association for the Advancement of Science (AAAS) in Science Advances
- Vol. 12 (28) , eaeh2106
Open AccessMechanical control of polar order
BiFeO 3 is a model multiferroic in which the ferroelectric polarization is coupled to ferroelastic lattice distortions, yet deterministic control of its domain structure remains limited by high switching fields and competing polarization variants. Here, we identify a mechanically assisted polarization switching pathway in epitaxial BiFeO 3 thin films that fundamentally alters the switching energetics. Using just out-of-plane electric fields, polarization reversal requires voltages of approximately 4 volts and stabilizes coexisting polarization states. In contrast, when mechanical pressure is applied concurrently, the positive coercive voltage can be substantially reduced, even to 0 volts, resulting in spontaneous switching. Piezoresponse force microscopy measurements reveal that applied mechanical pressure suppresses ferroelastic domain competition, indicating a decrease in the required electrical energy barrier associated with polarization rotation and domain wall motion. This frames the strain field from the AFM tip directly as an effective voltage that assists in ferroelectric switching. By directly coupling lattice distortions to polarization reversal, mechanically assisted switching provides a general framework for controlling coupled order parameters in multiferroic oxides, which can be directly applied in the device-level architecture, where a small mechanical pressure can help in achieving a lower switching energy of ferroelectric polarization. This work advances the fundamental understanding of electromechanical coupling in complex ferroics and establishes mechanical energy as a powerful tool for probing and manipulating ferroelastic-ferroelectric interactions.
- Open Access
- 7 July 2026
- Published by Springer Nature in Research Square
Vapor-Liquid-Liquid-Solid Synthesis of Single-Crystalline Weyl Semimetal NbP Nanowires with Reduced Resistivity
Weyl semimetals, characterized by topologically nontrivial band structures, exhibit unconventional transport properties and hold great promise for next-generation electronic devices. When reduced to the nanoscale, the contribution from the topological surface states becomes markedly enhanced, leading to unusual resistivity scaling behaviors. However, the synthesis of nanosized single-crystalline Weyl semimetals remains limited, hindering in-depth investigations of size-dependent transport phenomena. Here, we introduce a novel vapor-liquid-liquid-solid (VLLS) synthesis method for the growth of high-quality single-crystalline NbP nanowires with small diameters and controllable orientations. The VLLS process enables the stable and precise crystallization of NbP guided by Au seeds, favoring growth along the a axis, which has intrinsically lower resistivity. Room-temperature electrical measurements reveal a pronounced decrease in resistivity with decreasing diameter, indicating surface-dominant transport. We achieve a high breakdown current density of 116 MA cm –2 , comparable to that of copper nanowires, and a low resistivity of 21 µΩ cm at ~ 30 nm equivalent diameter, surpassing bulk NbP and many other semimetals. The dominance of topological surface states in charge transport is strongly supported by scanning microwave impedance microscopy measurements and simulations. The VLLS synthesis of NbP nanowires thus not only offers a pathway for precise structural control of Weyl semimetals but also opens new opportunities to tune their transport properties and enable advanced technological applications.
- 7 July 2026
- Published by Springer Nature in Research Square
Open AccessVapor-Liquid-Liquid-Solid Synthesis of Single-Crystalline Weyl Semimetal NbP Nanowires with Reduced Resistivity
Weyl semimetals, characterized by topologically nontrivial band structures, exhibit unconventional transport properties and hold great promise for next-generation electronic devices. When reduced to the nanoscale, the contribution from the topological surface states becomes markedly enhanced, leading to unusual resistivity scaling behaviors. However, the synthesis of nanosized single-crystalline Weyl semimetals remains limited, hindering in-depth investigations of size-dependent transport phenomena. Here, we introduce a novel vapor-liquid-liquid-solid (VLLS) synthesis method for the growth of high-quality single-crystalline NbP nanowires with small diameters and controllable orientations. The VLLS process enables the stable and precise crystallization of NbP guided by Au seeds, favoring growth along the a axis, which has intrinsically lower resistivity. Room-temperature electrical measurements reveal a pronounced decrease in resistivity with decreasing diameter, indicating surface-dominant transport. We achieve a high breakdown current density of 116 MA cm –2 , comparable to that of copper nanowires, and a low resistivity of 21 µΩ cm at ~ 30 nm equivalent diameter, surpassing bulk NbP and many other semimetals. The dominance of topological surface states in charge transport is strongly supported by scanning microwave impedance microscopy measurements and simulations. The VLLS synthesis of NbP nanowires thus not only offers a pathway for precise structural control of Weyl semimetals but also opens new opportunities to tune their transport properties and enable advanced technological applications.
- Open Access
- 12 May 2026
- Published by Springer Nature in Nature Communications
- Vol. 17 (1)
Room temperature molding of amorphous dielectrics via van der Waals anisotropy at the nanoscale
Mechanical instabilities produce periodic out-of-plane deformations, but applications remain limited by the need for elastic substrates and weak controllability. Here, we induce coherent, instability-driven buckling in both van der Waals (vdW) layers and underlying amorphous silica at room temperature, achieving precise spatial control and deterministic orientation. Electron-beam builds crystal-axis-dependent stress in α-MoO3, while simultaneously facilitating viscous flow in silica, producing sinusoidal wrinkles at subwavelength whose dimension are tunable by α-MoO3 thickness and electron dose. These wrinkles diffract light as on-chip optical gratings. We show coherent buckling across vdW heterostructures and peel off α-MoO3 post-buckling, leaving imprinted silica. Similar crystal-aligned wrinkles appear on amorphous Al2O3 and SiNx. By removing reliance on elastic substrates, this work extends the scope of instability-driven, lithography-free subwavelength patterning to CMOS-relevant dielectrics.
- 12 May 2026
- Published by Springer Nature in Nature Communications
- Vol. 17 (1)
Open AccessRoom temperature molding of amorphous dielectrics via van der Waals anisotropy at the nanoscale
Mechanical instabilities produce periodic out-of-plane deformations, but applications remain limited by the need for elastic substrates and weak controllability. Here, we induce coherent, instability-driven buckling in both van der Waals (vdW) layers and underlying amorphous silica at room temperature, achieving precise spatial control and deterministic orientation. Electron-beam builds crystal-axis-dependent stress in α-MoO3, while simultaneously facilitating viscous flow in silica, producing sinusoidal wrinkles at subwavelength whose dimension are tunable by α-MoO3 thickness and electron dose. These wrinkles diffract light as on-chip optical gratings. We show coherent buckling across vdW heterostructures and peel off α-MoO3 post-buckling, leaving imprinted silica. Similar crystal-aligned wrinkles appear on amorphous Al2O3 and SiNx. By removing reliance on elastic substrates, this work extends the scope of instability-driven, lithography-free subwavelength patterning to CMOS-relevant dielectrics.