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| Open AccessThermal dependence of the hydrated proton and optimal proton transfer in the protonated water hexamer
Water’s pivotal role is tied to the quantum nature of its hydrogen bond dynamics. Here, the authors investigate the thermal behavior of the protonated water hexamer through accurate path integral molecular dynamics, revealing that near-room temperature conditions are optimal for proton transfer.
- Félix Mouhat
- , Matteo Peria
- & Michele Casula
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Article
| Open AccessMulti-scale molecular dynamics simulations of enhanced energy transfer in organic molecules under strong coupling
Placing an organic material in an optical cavity can enhance exciton transport, but the mechanism is poorly understood. Here, using molecular dynamics simulations, the authors obtained atomistic insights into that mechanism.
- Ilia Sokolovskii
- , Ruth H. Tichauer
- & Gerrit Groenhof
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Article
| Open AccessAtomic high-spin cobalt(II) center for highly selective electrochemical CO reduction to CH3OH
Molecular catalysts provide an ideal model system to investigate the relationship between active site structure and catalytic performance. Here, the authors explore how electrochemical CO reduction to methanol can be controlled through modification of the active cobalt site in cobalt phthalocyanine.
- Jie Ding
- , Zhiming Wei
- & Bin Liu
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| Open AccessUniversal machine learning for the response of atomistic systems to external fields
External fields, despite their significant influence on chemical processes, have been largely ignored in current machine learning potentials. Here, the authors introduce a field-induced model that captures system-field interactions rigorously.
- Yaolong Zhang
- & Bin Jiang
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| Open AccessChirality-induced avalanche magnetization of magnetite by an RNA precursor
Homochirality, a key feature of life, has unknown origins. Magnetic mineral surfaces can act as chiral agents, but are only weakly magnetized by nature. Here, the authors report the uniform magnetization of magnetite by an RNA precursor that spreads across the surface like an avalanche.
- S. Furkan Ozturk
- , Deb Kumar Bhowmick
- & Dimitar D. Sasselov
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Article
| Open AccessInduced photoelectron circular dichroism onto an achiral chromophore
An achiral molecule can acquire a chiral spectroscopic signature when interacting with a chiral host. Here, the authors report the asymmetry in the electron distribution following ionisation of phenol complexed by chiral methyloxirane, which reflects an induced chirality onto the achiral phenol.
- Etienne Rouquet
- , Madhusree Roy Chowdhury
- & Anne Zehnacker
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Article
| Open AccessMachine learning electronic structure methods based on the one-electron reduced density matrix
Electronic structure methods are vital, yet they are often too computationally expensive. Here, the authors develop machine learned density matrices to fully represent electronic structures in a computationally cheap and accurate way.
- Xuecheng Shao
- , Lukas Paetow
- & Michele Pavanello
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| Open AccessStructure determination of ζ-N2 from single-crystal X-ray diffraction and theoretical suggestion for the formation of amorphous nitrogen
The ζ-N2 phase is key for comprehending the pressure-driven molecular to polymeric shift in nitrogen. Here, the authors resolved the crystal structure of ζ-N2 and identified a gradual delocalization of its electronic density under pressure, culminating in the initiation of nitrogen’s polymerization.
- Dominique Laniel
- , Florian Trybel
- & Natalia Dubrovinskaia
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Article
| Open AccessMending cracks atom-by-atom in rutile TiO2 with electron beam radiolysis
Radiolysis is known for damaging crystals. Here, using STEM, researchers observed radiolysis-driven bond-breakage, atomic movements, & crystal restructuring in rutile TiO2, and proposed a “2-step rolling” model of building blocks. These results open possibilities for constructive use of radiolysis.
- Silu Guo
- , Hwanhui Yun
- & K. Andre Mkhoyan
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Article
| Open AccessStrong structuring arising from weak cooperative O-H···π and C-H···O hydrogen bonding in benzene-methanol solution
Understanding liquid behavior is a challenge due to their disorder nature and rapid molecular rearrangements. Here, the authors show how weak interactions between OH groups and aromatic rings can participate in cooperative mechanisms that give rise to highly structured molecular arrangements in the liquid state.
- Camilla Di Mino
- , Andrew G. Seel
- & Neal T. Skipper
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Article
| Open AccessOrganic radical ferroelectric crystals with martensitic phase transition
Organic martensitic compounds are emerging smart materials with intriguing physical properties. Here authors show that upon H/F substitution a series of 1,4,5,8-naphthalenediimide derivatives exhibit reversible ferroelectric and martensitic transitions with a large thermal hysteresis.
- Nan Zhang
- , Wencong Sun
- & Han-Yue Zhang
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Article
| Open AccessDirected exciton transport highways in organic semiconductors
Optical properties of organic semiconductors enable various optoelectronic applications. Müller et al. report a large exciton bandwidth in a crystalline organic material and attribute it to the strong Coulomb interaction in directed exciton pathways induced by the donor–acceptor type molecular structure.
- Kai Müller
- , Karl S. Schellhammer
- & Frank Ortmann
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Article
| Open AccessDirectly imaging excited state-resolved transient structures of water induced by valence and inner-shell ionisation
Capturing the detailed structural evolution of electronic excited states is a challenging but critical step to understand and control ultrafast molecular dynamics. Here, combining a Coulomb explosion imaging approach and molecular dynamics simulations, the authors retrieve the transient geometry of the ground and excited states of D2O mono- and dication with few femtosecond, few picometre accuracy.
- Zhenzhen Wang
- , Xiaoqing Hu
- & Dajun Ding
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Article
| Open AccessEarly-stage bifurcation of crystallization in a sphere
Thermodynamics predicts equilibrium crystal structures and kinetics discover the pathway to form them. The authors investigate the interplay of thermodynamics and kinetics in the formation of colloidal clusters and reveal a bifurcation at an early stage of the crystallization process.
- Chrameh Fru Mbah
- , Junwei Wang
- & Michael Engel
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Article
| Open AccessSynthesis, structural analysis, and properties of highly twisted alkenes 13,13’-bis(dibenzo[a,i]fluorenylidene) and its derivatives
The rotation of a carbon double bond in an alkene can be efficiently accelerated by creating the high strain ground state and stabilizing the transition state of the process. Here, the authors report the synthesis, structures, and properties of several highly twisted alkenes.
- Hao-Wen Kang
- , Yu-Chiao Liu
- & Yao-Ting Wu
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Article
| Open AccessVisualization of π-hole in molecules by means of Kelvin probe force microscopy
A π-electron-deficient cavity in halogen-substituted polyaromatic hydrocarbon compounds, the so-called π-holes, have been predicted theoretically. Here authors present an experimental resolution of the πhole on a single molecule using the Kelvin probe force microscopy.
- B. Mallada
- , M. Ondráček
- & P. Jelínek
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Article
| Open AccessSpying on parahydrogen-induced polarization transfer using a half-tesla benchtop MRI and hyperpolarized imaging enabled by automation
Hyperpolarized magnetic resonance imaging (MRI) has the potential to revolutionize MRI applications, but requires large and clumsy instruments. Here, the authors present a 0.5 T benchtop system that allows to hyperpolarize, image, and spy on nuclear spins like 13C within seconds.
- Frowin Ellermann
- , Aidan Sirbu
- & Andrey N. Pravdivtsev
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| Open AccessImpact of hierarchical water dipole orderings on the dynamics of aqueous salt solutions
The behaviour of ions solvated in water is highly ion-specific. Introducing a length scale that captures the interplay between ion-water and inter-water interactions, along with considering the bond-orientational order of the hydration shell, provides an explanation for the ion-specific effects observed in salt solutions.
- Rui Shi
- , Anthony J. Cooper
- & Hajime Tanaka
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Article
| Open AccessEnantioselectivity of discretized helical supramolecule consisting of achiral cobalt phthalocyanines via chiral-induced spin selectivity effect
Experimental realizations of absolute enantioselection, without chiral catalysis or chiral ingredients, has been challenging. Here, the authors obtain enantioselectivity in mesoscale helical supramolecules consisting only of achiral molecules by exploiting chiral-induced spin selectivity (CISS) effect.
- Hiroki Aizawa
- , Takuro Sato
- & Hiroshi M. Yamamoto
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| Open AccessChirality control of a single carbene molecule by tip-induced van der Waals interactions
The control of molecular chirality is of great interest in stereochemistry and biochemistry. Here, the authors show how to alter the chirality dynamics of a single molecule through tip-induced van der Waals interactions.
- Yunjun Cao
- , Joel Mieres-Perez
- & Karina Morgenstern
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Article
| Open AccessEnhancing reactivity of SiO+ ions by controlled excitation to extreme rotational states
Control of chemical reactivity through excitation of rotational states is a relatively unexplored process that may play a role in interstellar chemistry. Here the authors show a marked acceleration of the hydrogen abstraction reaction between SiO+ and H2 by exciting super-rotor states of SiO+, in a joint experimental and theoretical study.
- Sruthi Venkataramanababu
- , Anyang Li
- & Brian C. Odom
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Article
| Open AccessAttosecond delays between dissociative and non-dissociative ionization of polyatomic molecules
The role of nuclear motion on photoionization delays is an interesting open question. Here the authors study photoionization delays in dissociative and non-dissociative ionization of a polyatomic molecule and explore the effect of isotopic substitution.
- Xiaochun Gong
- , Étienne Plésiat
- & Hans Jakob Wörner
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Article
| Open AccessSHARPER-DOSY: Sensitivity enhanced diffusion-ordered NMR spectroscopy
Since its discovery, the sensitivity of Nuclear Magnetic Resonance has increased steadily. Here the authors report on a liquid-state NMR methodology that increases the sensitivity of the diffusion coefficient measurements 10–100- fold, allowing to use microgram quantities of compounds, while reducing the measurement time to few minutes.
- George Peat
- , Patrick J. Boaler
- & Dušan Uhrín
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| Open AccessImpact of bimetallic interface design on heat generation in plasmonic Au/Pd nanostructures studied by single-particle thermometry
The conversion of light into heat is a key process for plasmonic-catalytic applications. Here, the authors investigate how the design of the bimetallic interface affects the photothermal heating properties in Au/Pd nanostructures by applying thermometry at the single-particle level.
- Julian Gargiulo
- , Matias Herran
- & Emiliano Cortés
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Article
| Open AccessStochastic representation of many-body quantum states
Variational approaches combined with machine learning are promising for solving quantum many-body problems, but they often suffer from scaling and optimization issues. Here the authors demonstrate that a stochastic representation of wavefunctions enables reducing the ground state search to standard regression.
- Hristiana Atanasova
- , Liam Bernheimer
- & Guy Cohen
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Article
| Open AccessMelting domain size and recrystallization dynamics of ice revealed by time-resolved x-ray scattering
The phase transition between water and ice is a ubiquitous phenomenon in nature. Here, the authors conduct a time-resolved x-ray scattering experiment using X-ray Free Electron Lasers to elucidate a comprehensive picture of the melting and recrystallization dynamics of crystalline ice, based on direct structural information.
- Cheolhee Yang
- , Marjorie Ladd-Parada
- & Kyung Hwan Kim
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Article
| Open AccessRevealing CO2 dissociation pathways at vicinal copper (997) interfaces
Catalytic CO2 dissociation pathways are selectively determined by surface geometry in heterogeneous catalysis. The authors find that the stepped Cu surfaces effectively affect CO2 activation in elementary reaction steps at the atomic level
- Jeongjin Kim
- , Youngseok Yu
- & Jeong Young Park
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| Open AccessDirect observation of coherence transfer and rotational-to-vibrational energy exchange in optically centrifuged CO2 super-rotors
In this work the authors use coherent anti-Stokes Raman scattering to study collisional vibrational excitation in highly rotationally excited CO2 molecules prepared in an optical centrifuge.
- Timothy Y. Chen
- , Scott A. Steinmetz
- & Christopher J. Kliewer
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Article
| Open AccessNonthermal acceleration of protein hydration by sub-terahertz irradiation
The collective intermolecular dynamics of protein and water molecules, which overlap in subterahertz frequencies, are relevant for protein function expressions. Here the authors develop highly sensitive dielectric measurements, revealing that protein hydration is nonthermally accelerated by sub-terahertz irradiation.
- Jun-ichi Sugiyama
- , Yuji Tokunaga
- & Masahiko Imashimizu
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Article
| Open AccessProbing the atomically diffuse interfaces in Pd@Pt core-shell nanoparticles in three dimensions
Deciphering the structure and composition of bimetallic nanomaterial interfaces is key to understanding their properties. Here, the authors investigate the diffuse interfaces in Pd@Pt core-shell nanoparticles in 3D using electron tomography with atomic resolution.
- Zezhou Li
- , Zhiheng Xie
- & Jihan Zhou
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Article
| Open AccessUnidirectional rotation of micromotors on water powered by pH-controlled disassembly of chiral molecular crystals
‘Molecular motors, fuelled by various physical and chemical means, can perform asymmetric linear and rotary motions that are inherently related to their asymmetric shapes. Here, the authors describe silver-organic micro-complexes of random shapes that exhibit macroscopic unidirectional rotation on water surface through the asymmetric release of cinchonine or cinchonidine chiral molecules.
- Itai Carmeli
- , Celine M. Bounioux
- & Shachar E. Richter
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Article
| Open AccessRehybridization dynamics into the pericyclic minimum of an electrocyclic reaction imaged in real-time
Electrocyclic reactions proceed through critical geometries, which are known as pericyclic transition states in thermal reactions and pericyclic minima in photochemical reactions. Here, the authors image the structure of a pericyclic minimum in real time using a combination of ultrafast electron diffraction and ab initio dynamics simulations.
- Y. Liu
- , D. M. Sanchez
- & T. J. A. Wolf
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Article
| Open AccessElectron diffraction of deeply supercooled water in no man’s land
Supercooled water in so-called “no man’s land” promises to reveal the origin of the water anomalies. Here, the authors use electron diffraction to provide the first characterization that spans this temperature range, which narrows down the array of possible explanations.
- Constantin R. Krüger
- , Nathan J. Mowry
- & Ulrich J. Lorenz
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| Open AccessMeasurement-induced collective vibrational quantum coherence under spontaneous Raman scattering in a liquid
Spontaneous Raman scattering is classically understood as an incoherent process. Here, the authors demonstrate that macroscopic quantum coherence among billions of vibrating molecules in a liquid is generated when single photon detection and single spatio-temporal mode excitation are implemented.
- Valeria Vento
- , Santiago Tarrago Velez
- & Christophe Galland
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Article
| Open AccessFlattened 1D fragments of fullerene C60 that exhibit robustness toward multi-electron reduction
Fullerenes are compelling molecular materials, but the reason for their high robustness to multi-electron reduction is still debated. Here, the authors synthesize flattened 1D fragments of fullerene C60 with high robustness against multi-electron reduction.
- Masahiro Hayakawa
- , Naoyuki Sunayama
- & Aiko Fukazawa
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Article
| Open AccessColloidal gelation with non-sticky particles
The colloidal composites of gel and solid inclusions are more commonly encountered in real life. Using simulations, authors identify two lengthscales whose interplay generically controls the gelation in composite gels.
- Yujie Jiang
- & Ryohei Seto
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Article
| Open AccessInelastic electron scattering induced quantum coherence in molecular dynamics
Photoabsorption and electron capture are known to induce quantum coherence in molecular dynamics. Here, the authors show that a non-resonant inelastic scattering of incoherent electrons induces such a coherence, which is the most general but hitherto unexplored way of triggering the coherent dynamics in a molecule.
- Akshay Kumar
- , Suvasis Swain
- & Vaibhav S. Prabhudesai
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| Open AccessQuantum dynamical effects of vibrational strong coupling in chemical reactivity
Experiments suggest that placing molecules in an infrared cavity alters their reactivity, an effect lacking a clear theoretical explanation. Here, the authors show that the key to understanding this process may lie in quantum light-matter interactions.
- Lachlan P. Lindoy
- , Arkajit Mandal
- & David R. Reichman
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Article
| Open AccessIn-plane and out-of-plane excitonic coupling in 2D molecular crystals
The mixing between Frenkel and charge-transfer characters in molecular excitons is difficult to analyze. Here, the authors demonstrate the onset and evolution of the mixing using 2D perylene molecular crystals by measuring the reorientation of emission transition dipoles with varying thicknesses.
- Dogyeong Kim
- , Sol Lee
- & Sunmin Ryu
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Article
| Open AccessSurface plasmon-enhanced photo-driven CO2 hydrogenation by hydroxy-terminated nickel nitride nanosheets
Plasmonic catalysts are often limited to Au, Ag, Cu, Al, etc. Now, hydroxy-terminated nickel nitride nanosheets are reported to be an alternative material for CO2 hydrogenation to CO using solar energy without co-catalysts or sacrificial agents.
- Saideep Singh
- , Rishi Verma
- & Vivek Polshettiwar
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Article
| Open AccessCondensation and asymmetric amplification of chirality in achiral molecules adsorbed on an achiral surface
The origin of homochirality in nature is an important but open question. Here, the authors provide insight into the physicochemical origin of homochirality through surface adsorption on the model of adlayers of achiral carbon monoxide molecules on an achiral Au(111) surface.
- Huiru Liu
- , Heping Li
- & Lan Chen
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Article
| Open AccessTowards the ground state of molecules via diffusion Monte Carlo on neural networks
An accurate ab initio calculation of molecules is fundamental to chemical and physical sciences. Here, the authors integrate a neural-network wavefunction into the fixed-node diffusion Monte Carlo, resulting in accurate calculations of a diverse range of systems, offering insights into complex many-body electronic wave functions.
- Weiluo Ren
- , Weizhong Fu
- & Ji Chen
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Article
| Open AccessHyperloop-like diffusion of long-chain molecules under confinement
Normally, the diffusion of the object is suppressed in the confined space. Here, by regulating the degrees of freedom of the molecule, authors demonstrate ultrafine diffusion in the sub-nano space.
- Jiamin Yuan
- , Mingbin Gao
- & Anmin Zheng
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Article
| Open AccessThe critical role of ultra-low-energy vibrations in the relaxation dynamics of molecular qubits
Understanding phonon-induced relaxation in molecular qubits is a crucial step in realizing their application potential. Garlatti at al. use a combination of inelastic X-ray scattering and density functional theory to investigate the role of low-energy phonons on spin relaxation of a prototypical molecular qubit.
- E. Garlatti
- , A. Albino
- & S. Carretta
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Article
| Open AccessRapid handheld time-resolved circularly polarised luminescence photography camera for life and material sciences
Despite their high brightness and long-lived emission, lanthanide based circularly polarised luminophores have not been fully exploited for real-life application. Here, the authors present an all solid-state circularly polarised luminescence camera to facilitate ad hoc time-resolved enantioselective differential chiral contrast-based one-shot photography that can be applied in life and material sciences.
- Davide F. De Rosa
- , Patrycja Stachelek
- & Robert Pal
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Article
| Open AccessVisualizing defect dynamics by assembling the colloidal graphene lattice
Colloidal particles bonding via attractive patches mimic the bonding of atoms in atomic compounds and materials. By assembling patchy particles into the graphene lattice, the authors obtain insight into lattice defects in this important 2D material.
- Piet J. M. Swinkels
- , Zhe Gong
- & Peter Schall
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Article
| Open AccessThe collective burst mechanism of angular jumps in liquid water
The collective nature of reorientational dynamics in water remains poorly understood. Here, the authors show that large angular fluctuations require a highly cooperative dynamics involving correlated motion of many water molecules in the hydrogen-bond network that form spatially connected clusters.
- Adu Offei-Danso
- , Uriel N. Morzan
- & Asja Jelic
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Article
| Open AccessTransient dynamics of the phase transition in VO2 revealed by mega-electron-volt ultrafast electron diffraction
The atomic pathway in the photoinduced ultrafast structural phase transition of VO2 has been a controversial problem for a long time. Here the authors, using MeV ultrafast electron diffraction, show that the melting of V-V dimers and the transformation of crystal symmetry are two processes with different timescales.
- Chenhang Xu
- , Cheng Jin
- & Dong Qian
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Article
| Open AccessEntangled spin-polarized excitons from singlet fission in a rigid dimer
Singlet fission is recognized as an enabling process for next-generation solar cells. Here the authors design a molecular system where specific spin sub-levels can be initialized to produce a highly entangled state and demonstrate that the coherence between magnetic sub-levels of that state is preserved at higher temperatures than those encountered in conventional superconducting quantum hardware.
- Ryan D. Dill
- , Kori E. Smyser
- & Joel D. Eaves