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Moiré superlattices have led to observations of exotic emergent electronic properties such as superconductivity and strong correlated states in small-rotation-angle twisted bilayer graphene (tBLG)

The recent discovery of natural biaxial hyperbolicity in van der Waals crystals, such as α-MoO3, has opened up new avenues for mid-IR nanophotonics due to their deep subwavelength phonon polaritons. However, a significant challenge is the lack of active tunability of these hyperbolic phonon polaritons. In this work, we investigate heterostructures of graphene and α-MoO3 for actively tunable hybrid plasmon phonon polariton modes via electrostatic gating in the mid-infrared spectral region. We observe a unique propagation direction dependent hybridization of graphene plasmon polaritons with hyperbolic phonon polaritons for experimentally feasible values of graphene chemical potential. We further report an application to tunable valley quantum interference in this system with a broad operational bandwidth due to the formation of these hybrid modes. This work presents a lithography-free alternative for actively tunable, anisotropic spontaneous emission enhancement using a sub-wavelength thick naturally biaxial hyperbolic material.

Perpendicular magnetic tunnel junctions (p-MTJs) switched utilizing bipolar electric fields have extensive applications in energy-efficient memory and logic devices. Voltage-controlled magnetic anisotropy linearly lowers the energy barrier of the ferromagnetic layer via the electric field effect and efficiently switches p-MTJs only with a unipolar behavior. Here, we demonstrate a bipolar electric field effect switching of 100 nm p-MTJs with a synthetic antiferromagnetic free layer through voltage-controlled exchange coupling (VCEC). The switching current density, ∼1.1 × 10

Transition metal dichalcogenide (TMD) layered semiconductors possess immense potential in the design of photonic, electronic, optoelectronic, and sensor devices. However, sub-bandgap light absorption of TMD in the range from near-infrared (NIR) to short-wavelength infrared (SWIR) is insufficient for applications beyond the bandgap limit. Herein, we report that the sub-band photoresponse of MoS2 /Au heterostructures can be robustly modulated by the electrode fabrication method employed. We observed up to 60% sub-bandgap absorption in the MoS2 /Au heterostructure, which includes the hybridized interface, where the Au layer was applied via sputter deposition. The greatly enhanced absorption of sub-bandgap light is due to the planar cavity formed by MoS2 and Au; as such, the absorption spectrum can be tuned by altering the thickness of the MoS2 layer. Photocurrent in the SWIR wavelength range increases due to increased SWIR absorption, which means that broad wavelength detection from visible toward SWIR is possible. We also achieved rapid photoresponse (~ 164 µs) and high responsivity (17 mA W− 1) at an excitation wavelength of 1,550 nm. Our findings here demonstrate a facile method for optical property modulation using metal electrode engineering and for realizing SWIR photodetection in wide-bandgap 2D materials.

We proposed a mechanism to generate giant anisotropic second harmonic nonlinear response via double resonance effect, achieved through band nesting via electronic bandstructure engineering. The ideal band setup would be a triplet of nested bands separated by the fundamental resonance energy, $\hbar\omega$. We demonstrate theoretically that the proposed phenomenon can be realized in bilayer SnS by band tuning with perpendicular electrical bias, which maximizes the second harmonic susceptibility by several orders of magnitude. Moreover, the tunability of the polarization anisotropy can be useful for realizing novel polarization-sensitive devices.

The coupling of plasmons and vibrational modes has been routinely observed in graphene and other 2D systems in both near-field and far-field spectroscopy. However, the relation between coupling str...

Monolayer transition metal dichalcogenides are promising materials for spintronics due to their robust spin-valley locked valence states, enabling efficient charge-to-spin conversion via valley Hall effect with non-equilibrium spins possessing long spin diffusion lengths of hundreds of nanometers. In this work, we show that the injection of a pure valley current, induced by valley Hall effect in a WSe2 monolayer, imparts a spin torque on the magnetization of an overlaid Fe or CoFe in a tunneling structure. The torque efficiency is found to be comparable to that in conventional perpendicular magnetic tunnel junctions and can be further optimized with valley Hall angle in WSe2. The valley nature of the spin torque gives rise to out-of-plane damping-like torques in a current-in-plane configuration, vanishing charge transport perpendicular-to-the-plane as well as torque efficiency tunable through gating.

The lack of certain crystalline symmetries in strong spin-orbit-coupled non-magnetic materials allows for the existence of uncoventional spin Hall responses, with electrically generated transverse spin currents possessing collinear flow and spin directions. The injection of such spin currents into an adjacent ferromagnetic layer can excite magnetization dynamics via unconventional spin-orbit torques, leading to deterministic switching in ferromagnets with perpendicular magnetic anisotropy. We study the interplay between conventional and unconventional spin-orbit torques on the magnetization dynamics of a perpendicular ferromagnet in the small intrinsic damping limit, and identify a rich set of dynamical regimes that includes deterministic and probabilistic switching, precessional and pinning states. Contrary to common belief, we found that there exists a critical conventional spin Hall angle, beyond which deterministic magnetization switching transitions to a precessional or pinned state. Conversely, we showed that larger unconventional spin Hall angle is generally beneficial for deterministic switching. We derive an approximate expression that qualitatively describes the state diagram boundary between the full deterministic switching and precessional states and discuss a criterion for searching symmetry-broken spin Hall materials in order to maximize switching efficiency. Our work offers a roadmap towards energy efficient spintronic devices, which might opens doors for applications in advanced in-memory computing technologies.

In the course of searching for promising topological materials for applications in future topological electronics, we evaluated spin-orbit torques (SOTs) in high-quality sputtered ${\delta}-$TaN/Co20Fe60B20 devices through spin-torque ferromagnetic resonance ST-FMR and spin pumping measurements. From the ST-FMR characterization we observed a significant linewidth modulation in the magnetic Co20Fe60B20 layer attributed to the charge-to-spin conversion generated from the ${\delta}-$TaN layer. Remarkably, the spin-torque efficiency determined from ST-FMR and spin pumping measurements is as large as ${\Theta} =$ 0.034 and 0.031, respectively. These values are over two times larger than for ${\alpha}-$Ta, but almost five times lower than for ${\beta}-$Ta, which can be attributed to the low room temperature electrical resistivity $\sim 74{\mu}{\Omega}$ cm in ${\delta}-$TaN. A large spin diffusion length of at least $\sim8$ nm is estimated, which is comparable to the spin diffusion length in pure Ta. Comprehensive experimental analysis, together with density functional theory calculations, indicates that the origin of the pronounced SOT effect in ${\delta}-$TaN can be mostly related to a significant contribution from the Berry curvature associated with the presence of a topically nontrivial electronic band structure in the vicinity of the Fermi level (EF). Through additional detailed theoretical analysis, we also found that an isostructural allotrope of the superconducting ${\delta}-$TaN phase, the simple hexagonal structure, ${\theta}-$TaN, has larger Berry curvature, and that, together with expected reasonable charge conductivity, it can also be a promising candidate for exploring a generation of spin-orbit torque magnetic random access memory as cheap, temperature stable, and highly efficient spin current sources., Comment: 28 pages, 7 figures

Near-field mapping has been widely used to study hyperbolic phonon-polaritons in van der Waals crystals. However, an accurate measurement of the polaritonic loss remains challenging because of the inherent complexity of the near-field signal and the substrate-mediated loss. Here we demonstrate that large-area monocrystalline gold flakes, an atomically flat low-loss substrate for image polaritons, provide a platform for precise near-field measurement of the complex propagation constant of polaritons in van der Waals crystals. As a topical example, we measure propagation loss of the image phonon-polaritons in hexagonal boron nitride, revealing that their normalized propagation length exhibits a parabolic spectral dependency. Furthermore, we show that image phonon-polaritons exhibit up to a twice longer normalized propagation length, while being 2.4 times more compressed compared to the case of the dielectric substrate. We conclude that the monocrystalline gold flakes provide a unique nanophotonic platform for probing and exploitation of the image modes in low-dimensional materials.

Atomically thin materials can be used to build novel forms of conventional semiconductor heterostructure devices. One such device is a resonant tunnelling diode, which can exhibit negative differential resistance and usually consists of a quantum-well structure between two barrier layers. Here, we show that a twisted black phosphorus homostructure can be used to create a resonant tunnelling diode. The devices have a trilayer structure in which a thin non-degenerate black phosphorus layer is sandwiched between two thicker degenerate black phosphorus layers. The interlayer coupling strength depends sensitively on the twist angle between the layers, and thus the twist angle can be used to control the vertical transport behaviour, from ohmic to tunnelling. Because resonant tunnelling through quantum-well states occurs without the need for a physical tunnelling barrier, our devices exhibit a higher tunnelling conductance and negative differential resistance peak-to-valley current ratio than resonant tunnelling diodes based on van der Waals heterostructures. Twisted trilayer structures of anisotropic black phosphorus can be used to create resonant tunnelling diodes in which the twist angle between the layers can be used to control the vertical transport behaviour.

An acoustic plasmon mode in a graphene-dielectric-metal structure has recently been spotlighted as a superior platform for strong light-matter interaction. It originates from the coupling of graphene plasmon with its mirror image and exhibits the largest field confinement in the limit of a sub-nm-thick dielectric. Although recently detected in the far-field regime, optical near-fields of this mode are yet to be observed and characterized. Here, we demonstrate a direct optical probing of the plasmonic fields reflected by the edges of graphene via near-field scattering microscope, revealing a relatively small propagation loss of the mid-infrared acoustic plasmons in our devices that allows for their real-space mapping at ambient conditions even with unprotected, large-area graphene grown by chemical vapor deposition. We show an acoustic plasmon mode that is twice as confined and has 1.4 times higher figure of merit in terms of the normalized propagation length compared to the graphene surface plasmon under similar conditions. We also investigate the behavior of the acoustic graphene plasmons in a periodic array of gold nanoribbons. Our results highlight the promise of acoustic plasmons for graphene-based optoelectronics and sensing applications., Acoustic graphene plasmons are superior to the graphene surface plasmons in field confinement and normalized propagation length, thus promising for applications. Here, the authors report near-field imaging of acoustic plasmons in high-quality CVD graphene, measure the AGP dispersion and propagation loss, and investigate their behavior in a periodic structure.

We investigate the twist angle dependence of spin-orbit coupling (SOC) proximity effects and charge-to-spin conversion (CSC) in graphene/WSe$_2$ heterostructures from first principles. The CSC is shown to strongly depend on the twist angle, with both the spin Hall and standard Rashba-Edelstein efficiencies optimized at or near 30{\deg} twisting. Symmetry breaking due to twisting also gives rise to an unconventional Rashba-Edelstein effect, with electrically generated non-equilibrium spin densities possessing spins collinear to the applied electric field. We further discuss how the carrier doping concentration and band broadening control the crossover between the Fermi-sea and -surface spin response, which reconciles the seemingly disparate experimental observations of different CSC phenomena., Comment: 5 pages, 4 figures, Supplementary Information (13 pages, 7 figures)

The ability to control the light polarization state is critically important for diverse applications in information processing, telecommunications, and spectroscopy. Here, we propose that a stack of anisotropic van der Waals materials can facilitate the building of optical elements with Jones matrices of unitary, Hermitian, non-normal, singular, degenerate, and defective classes. We show that the twisted stack with electrostatic control can function as arbitrary-birefringent wave-plate or arbitrary polarizer with tunable degree of non-normality, which in turn give access to plethora of polarization transformers including rotators, pseudorotators, symmetric and ambidextrous polarizers. Moreover, we discuss an electrostatic-reconfigurable stack which can be tuned to operate as four different polarizers and be used for Stokes polarimetry., K. K and T.L. acknowledge partial support by the National Science Foundation, NSF/EFRI Grant No. EFRI-1741660, and the DDF UMN support for K. K.LM-MacknowledgesProjectPID2020-115221GB-C41 financed by MCIN/AEI/10.13039/501100011033 and the Aragon Government through Project Q-MAD. S.-H.O. acknowledges support from the Samsung Global Research (GRO) Program and the Sanford P. Bordeau Chair at the University of Minnesota.

Electrostatically defined quantum dots (QDs) in Bernal stacked bilayer graphene (BLG) are a promising quantum information platform because of their long spin decoherence times, high sample quality, and tunability. Importantly, the shape of QD states determines the electron energy spectrum, the interactions between electrons, and the coupling of electrons to their environment, all of which are relevant for quantum information processing. Despite its importance, the shape of BLG QD states remains experimentally unexamined. Here we report direct visualization of BLG QD states by using a scanning tunneling microscope. Strikingly, we find these states exhibit a robust broken rotational symmetry. By using a numerical tight-binding model, we determine that the observed broken rotational symmetry can be attributed to low energy anisotropic bands. We then compare confined holes and electrons and demonstrate the influence of BLG's nontrivial band topology. Our study distinguishes BLG QDs from prior QD platforms with trivial band topology.

Polaritons in two-dimensional materials provide extreme light confinement that is difficult to achieve with metal plasmonics. However, such tight confinement inevitably increases optical losses through various damping channels. Here we demonstrate that hyperbolic phonon polaritons in hexagonal boron nitride can overcome this fundamental trade-off. Among two observed polariton modes, featuring a symmetric and antisymmetric charge distribution, the latter exhibits lower optical losses and tighter polariton confinement. Far-field excitation and detection of this high-momenta mode become possible with our resonator design that can boost the coupling efficiency via virtual polariton modes with image charges that we dub ‘image polaritons’. Using these image polaritons, we experimentally observe a record-high effective index of up to 132 and quality factors as high as 501. Further, our phenomenological theory suggests an important role of hyperbolic surface scattering in the damping process of hyperbolic phonon polaritons., The tight confinement of polaritons in 2D materials leads to increased optical losses. Here, the authors demonstrate image phonon polariton modes in hexagonal boron nitride with an antisymmetric charge distribution that feature quality factors of up to 501 and an effective index of 132.

In integrated photonics, specific wavelengths such as 1,550 nm are preferred due to low-loss transmission and the availability of optical gain in this spectral region. For chip-based photodetectors, two-dimensional materials bear scientifically and technologically relevant properties such as electrostatic tunability and strong light–matter interactions. However, no efficient photodetector in the telecommunication C-band has been realized with two-dimensional transition metal dichalcogenide materials due to their large optical bandgaps. Here we demonstrate a MoTe2-based photodetector featuring a strong photoresponse (responsivity 0.5 A W–1) operating at 1,550 nm in silicon photonics enabled by strain engineering the two-dimensional material. Non-planarized waveguide structures show a bandgap modulation of 0.2 eV, resulting in a large photoresponse in an otherwise photoinactive medium when unstrained. Unlike graphene-based photodetectors that rely on a gapless band structure, this photodetector shows an approximately 100-fold reduction in dark current, enabling an efficient noise-equivalent power of 90 pW Hz–0.5. Such a strain-engineered integrated photodetector provides new opportunities for integrated optoelectronic systems. A strain-induced absorption-enhanced MoTe2-based silicon photonic microring-integrated photodetector is demonstrated, featuring high responsivity of ~0.5 A W–1 at 1,550 nm, with a low noise-equivalent power of 90 pW Hz–0.5.

Topological properties of the Lieb lattice, i.e., the edge-centered square lattice, have been extensively studied and are, however, mostly based on theoretical models without identifying real material systems. Here, based on tight-binding and first-principles calculations, we demonstrate the Lieb-lattice features of the experimentally synthesized phthalocyanine-based metal-organic framework (MPc-MOF), which holds various intriguing topological phase transitions through band engineering. First, we show that the MPc-MOFs indeed have a peculiar Lieb band structure with 1/3 filling, which has been overlooked because of its unconventional band structure deviating from the ideal Lieb band. The intrinsic MPc-MOF presents a trivial insulating state, with its gap size determined by the on-site energy difference (ΔE) between the corner and edge-center sites. Through either chemical substitution or physical strain engineering, one can tune ΔE to close the gap and achieve a topological phase transition. Specifically, upon closing the gap, topological semimetallic/insulating states emerge from nonmagnetic MPc-MOFs, while magnetic semimetal/Chern insulator states arise from magnetic MPc-MOFs, respectively. Our discovery greatly enriches our understanding of the Lieb lattice and provides a guideline for experimental observation of the Lieb-lattice-based topological states.

Dynamic high-resolution wavefront modulation of light is a long-standing quest in photonics. Metasurfaces have shown potential for realizing light manipulation with subwavelength resolution through nanoscale optical elements, or metaatoms, to overcome the limitations of conventional spatial light modulators. State-of-the-art active metasurfaces operate via phase modulation of the metaatoms, and their inability to also independently control the scattered amplitude leads to an inferior reconstruction of the desired wavefronts. This fundamental problem posed severe performance limitations particularly for applications relying on subwavelength spatiotemporal complex field modulation, which includes dynamic holography, high-resolution imaging, optical tweezing, and optical information processing. Here, we present the "metamolecule" strategy, which incorporates two independent subwavelength scatterers composed of noble metal antennas coupled to gate-tunable graphene plasmonic nanoresonators. The two-parametric control of the metamolecule secures the complete control of both amplitude and phase of light, enabling 2π phase shift as well as large amplitude modulation including perfect absorption. We further develop a generalized graphical model to examine the underlying requirements for complete complex amplitude modulation, offering intuitive design guidelines to maximize the tunability in metasurfaces. To illustrate the reconfigurable capability of our designs, we demonstrate dynamic beam steering and holographic wavefront reconstruction in periodically arranged metamolecules.

Indium Selenide (In2Se3) is a newly emerged van der Waals (vdW) ferroelectric material, which unlike traditional insulating ferroelectric materials, is a semiconductor with a bandgap of about 1.36 eV. Ferroelectric diodes and transistors based on In2Se3 have been demonstrated. However, the interplay between light and electric polarization in In2Se3 has not been explored. In this paper, we found that the polarization in In2Se3 can be programmed by optical stimuli, due to its semiconducting nature, where the photo generated carriers in In2Se3 can alter the screening field and lead to polarization reversal. Utilizing these unique properties of In2Se3, we demonstrated a new type of multifunctional device based on 2D heterostructures, which can concurrently serve as a logic gate, photodetector, electronic memory and photonic memory. This dual electrical and optical operation of the memories can simplify the device architecture and offer additional functionalities, such as ultrafast optical erase of large memory arrays. In addition, we show that dual-gate structure can address the partial switching problem commonly observed in In2Se3 ferroelectric transistors, as the two gates can enhance the vertical electric field and facilitate the polarization switching in the semiconducting In2Se3. These discovered effects are of general nature and should be observable in any ferroelectric semiconductor. These findings deepen the understanding of polarization switching and light-polarization interaction in semiconducting ferroelectric materials and open up their applications in multifunctional electronic and photonic devices.

Photonic spin Hall effect is a manifestation of spin-orbit interaction of light and can be measured by a transverse shift \lambda of photons with opposite spins. The precise measurement of transverse shifts can enable many spin-related applications, such as precise metrology and optical sensing. However, this transverse shift is generally small (i.e. \delta /\lambda {10}^{2}) have severe limitations, particularly its occurrence only over a narrow angular cone (with a width of \Delta \theta {70}^{\circ} by exploiting the interface between free space and uniaxial epsilon-near-zero media. The underlying mechanism is ascribed to the almost-perfect polarization splitting between s and p polarized waves at the designed interface. Remarkably, this almost-perfect polarization splitting does not resort to the interference effect and is insensitive to the incident angle, which then gives rise to the wide-angle giant photonic spin Hall effect., Comment: 18 pages, 9 figures

While nature provides a plethora of perovskite materials, only a few exhibit large ferroelectricity and possibly multiferroicity. The majority of perovskite materials have the nonpolar CaTiO_{3}(CTO) structure, limiting the scope of their applications. Based on the effective Hamiltonian model as well as first-principles calculations, we propose a general thin-film design method to stabilize the functional BiFeO_{3}(BFO)-type structure, which is a common metastable structure in widespread CTO-type perovskite oxides. It is found that the improper antiferroelectricity in CTO-type perovskite and ferroelectricity in BFO-type perovskite have distinct dependences on mechanical and electric boundary conditions, both of which involve oxygen octahedral rotation and tilt. The above difference can be used to stabilize the highly polar BFO-type structure in many CTO-type perovskite materials., This work was supported by National Science Foundation through Grants No. DMR-2053195 (X. W.). H. W. was partially supported as part of the Center for the Computational Design of Functional Layered Materials, Department of Energy, Office of Science, Basic Energy Sciences, under Grant No. DE-SC0012575. T. L. acknowledges funding support from NSF=DMREF under Grant Agreement No. 1921629. Q. A. was supported by the American Chemical Society Petroleum Research Fund (PRF No. 58754-DNI6). The computational work used resources of the National Energy Research Scientific Computing Center (NERSC), a U.S. Department of Energy Office of Science User Facility operated under Contract No. DE-AC02-05CH11231., With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2019-000917-S).

Two-dimensional half-metallicity without a transition metal is an attractive attribute for spintronics applications. On the basis of first-principles calculation, we revealed that a two-dimensional gallium nitride (2D-GaN), which was recently synthesized between graphene and SiC or wurtzite GaN substrate, exhibits half-metallicity due to its half-filled quasi-flat band. We found that graphene plays a crucial role in stabilizing a local octahedral structure, whose unusually high density of states due to a flat band leads to a spontaneous phase transition to its half-metallic phase from normal metal. It was also found that its half-metallicity is strongly correlated to the in-plane lattice constants and thus subjected to substrate modification. To investigate the magnetic property, we simplified its magnetic structure with a two-dimensional Heisenberg model and performed Monte Carlo simulation. Our simulation estimated its Curie temperature (

The rapid discovery of two-dimensional (2D) van der Waals (vdW) quantum materials has led to heterostructures that integrate diverse quantum functionalities such as topological phases, magnetism, and superconductivity. In this context, the epitaxial synthesis of vdW heterostructures with well-controlled interfaces is an attractive route towards wafer-scale platforms for systematically exploring fundamental properties and fashioning proof-of-concept devices. Here, we use molecular beam epitaxy to synthesize a vdW heterostructure that interfaces two material systems of contemporary interest: a 2D ferromagnet (1T-CrTe

Topological spin textures are field arrangements that cannot be continuously deformed to a fully polarized state. In particular, merons are topological textures characterized by half-integer topological charge ±1/2 and vortex-like swirling patterns at large distances. Merons have been studied previously in the context of cosmology, fluid dynamics, condensed matter physics and plasmonics. Here, we visualized optical spin angular momentum of phonon polaritons that resembles nanoscale meron spin textures. Phonon polaritons, hybrids of infrared photons and phonons in hexagonal boron nitride, were excited by circularly polarized light incident on a ring-shaped antenna and imaged using infrared near-field techniques. The polariton field reveals a half-integer topological charge determined by the handedness of the incident beam. Our phonon polaritonic platform opens up new pathways to create, control, and visualize topological textures.

Non-reciprocal plasmons in current-driven, isotropic, and homogenous graphene with proximal metallic gates is theoretically explored. Nearby metallic gates screen the Coulomb interactions, leading to linearly dispersive acoustic plasmons residing close to its particle-hole continuum counterpart. We show that the applied bias leads to spectral broadband focused plasmons whose resonance linewidth is dependent on the angular direction relative to the current flow due to Landau damping. We predict that forward focused non-reciprocal plasmons are possible with accessible experimental parameters and setup.

Transition metal dichalcogenides (TMDCs) and two-dimensional organic and inorganic hybrid lead halide perovskites (2DPVSKs) have emerged as highly promising materials for ultralight and ultrathin optoelectronics application. They both exhibit tunability of electronic properties such as band structure, and they can form heterostructures with various types of two-dimensional materials for novel physical properties not observed in single components. However, TMDCs exhibit poor emission efficiency due to defect states and direct-to-indirect interband transition, and 2DPVSKs suffer from poor stability in ambient atmosphere. Here we report that fabrication of TMDC-on-2DPVSK heterostructures using a solvent-free process leads to novel optical transitions unique to the heterostructure which arise from the hybrid interface and exhibit a strong photoluminescence. Moreover, a two orders of magnitude enhancement of the photoluminescence as compared to WS2 emission is observed. The TMDC on top of 2DPVSK also significantly improves the stability as compared to bare 2DPVSK. Enhanced emission can be explained by electronic structure modification of TMDC by novel interfacial interactions between TMDC and 2DPVSK materials, which shows promise of the heterostructure for high efficiency and stable optoelectronic devices.

One of the fundamental hurdles in plasmonics is the trade-off between electromagnetic field confinement and the coupling efficiency with free-space light, a consequence of the large momentum mismatch between the excitation source and plasmonic modes. Acoustic plasmons in graphene, in particular, have an extreme level of field confinement, as well as an extreme momentum mismatch. Here, we show that this fundamental compromise can be overcome and demonstrate a graphene acoustic plasmon resonator with nearly perfect absorption (94%) of incident mid-infrared light. This high efficiency is achieved by utilizing a two-stage coupling scheme: free-space light coupled to conventional graphene plasmons, which then couple to ultraconfined acoustic plasmons. To realize this scheme, we transfer unpatterned large-area graphene onto template-stripped ultraflat metal ribbons. A monolithically integrated optical spacer and a reflector further boost the enhancement. We show that graphene acoustic plasmons allow ultrasensitive measurements of absorption bands and surface phonon modes in angstrom-thick protein and SiO2 layers, respectively. Our acoustic plasmon resonator platform is scalable and can harness the ultimate level of light-matter interactions for potential applications including spectroscopy, sensing, metasurfaces and optoelectronics.