Compartmentalization in living systems,where multiple reactions occur in parallel within confined spaces,has inspired the development of droplet networks in the past decade.These fascinating assemblies offer unique an...Compartmentalization in living systems,where multiple reactions occur in parallel within confined spaces,has inspired the development of droplet networks in the past decade.These fascinating assemblies offer unique and versatile functions that are unattainable by single droplets and have shown their potential as advanced platforms for chemical and biological applications.This review highlights recent progress in the creation and application of droplet networks,covering strategies for generating the droplets and assembling them into functional networks.Key applications such as microreactors,signal conductors,actuators,and power sources are summarized.We also discuss the challenges and future trends in this field,aiming to narrow the gap between fundamental research and real applications.展开更多
Molecular conformation is crucial to its chemical reactivity,1,2 electron transport,3,4 and photophysical properties.5 However,it is very challenging to precisely control,as molecules typically switch rapidly between ...Molecular conformation is crucial to its chemical reactivity,1,2 electron transport,3,4 and photophysical properties.5 However,it is very challenging to precisely control,as molecules typically switch rapidly between different conformations,which are generally considered to be in thermal equilibrium.This is especially true in multiphenyl systems,where conformational changes induced byσ-bond rotations are both complex and rapid,6,7 making it very challenging to precisely monitor and control conformational switching at thesingle-molecule level.展开更多
Quantum computers(QC)could harbor the potential to significantly advance materials simulations,particularly at the atomistic scale involving strongly correlated fermionic systems,where an accurate description of quant...Quantum computers(QC)could harbor the potential to significantly advance materials simulations,particularly at the atomistic scale involving strongly correlated fermionic systems,where an accurate description of quantummany-body effects scales unfavorably with size.While a full-scale treatment of condensed matter systems with currently available noisy quantum computers remains elusive,quantum embedding schemes like dynamical mean-field theory(DMFT)allow the mapping of an effective,reduced subspace Hamiltonian to available devices to improve the accuracy of ab initio calculations such as density functional theory(DFT).Here,we report on the development of a hybrid quantum-classical DFT+DMFT simulation framework which relies on a quantum impurity solver based on the Lehmann representation of the impurity Green’s function.Hardware experiments with up to 14 qubits on the IBM Quantum system are conducted,using advanced error mitigation methods and a novel calibration scheme for an improved zero-noise extrapolation to effectively reduce adverse effects from inherent noise on current quantum devices.We showcase the utility of our quantum DFT+DMFT workflow by assessing the correlation effects on the electronic structure of a real material,Ca_(2)CuO_(2)Cl_(2),which is mapped to an effective single-band Hubbard Hamiltonian and the subsequently derived Anderson impurity model solved with up to 6 bath sites on available quantum hardware.Further,we carefully benchmark our quantum results with respect to exact reference solutions and experimental spectroscopy measurements.While challenges remain to scale our approach to larger,multi-orbital and multi-site systems with more bath sites,the present work marks an important milestone towards achieving utility-scale quantum computation in materials simulation.展开更多
基金National Science Foundation of China,Grant/Award Numbers:52033002,22372032,22202040Natural Science Foundation of Jiangsu Province,Grant/Award Number:BK20211560Young Elite Scientists Sponsorship Programby CAST,Grant/Award Number:2022QNRC001。
文摘Compartmentalization in living systems,where multiple reactions occur in parallel within confined spaces,has inspired the development of droplet networks in the past decade.These fascinating assemblies offer unique and versatile functions that are unattainable by single droplets and have shown their potential as advanced platforms for chemical and biological applications.This review highlights recent progress in the creation and application of droplet networks,covering strategies for generating the droplets and assembling them into functional networks.Key applications such as microreactors,signal conductors,actuators,and power sources are summarized.We also discuss the challenges and future trends in this field,aiming to narrow the gap between fundamental research and real applications.
文摘Molecular conformation is crucial to its chemical reactivity,1,2 electron transport,3,4 and photophysical properties.5 However,it is very challenging to precisely control,as molecules typically switch rapidly between different conformations,which are generally considered to be in thermal equilibrium.This is especially true in multiphenyl systems,where conformational changes induced byσ-bond rotations are both complex and rapid,6,7 making it very challenging to precisely monitor and control conformational switching at thesingle-molecule level.
基金support from the German Federal Ministry of Education and Research (BMBF) under project No. 13N15574.
文摘Quantum computers(QC)could harbor the potential to significantly advance materials simulations,particularly at the atomistic scale involving strongly correlated fermionic systems,where an accurate description of quantummany-body effects scales unfavorably with size.While a full-scale treatment of condensed matter systems with currently available noisy quantum computers remains elusive,quantum embedding schemes like dynamical mean-field theory(DMFT)allow the mapping of an effective,reduced subspace Hamiltonian to available devices to improve the accuracy of ab initio calculations such as density functional theory(DFT).Here,we report on the development of a hybrid quantum-classical DFT+DMFT simulation framework which relies on a quantum impurity solver based on the Lehmann representation of the impurity Green’s function.Hardware experiments with up to 14 qubits on the IBM Quantum system are conducted,using advanced error mitigation methods and a novel calibration scheme for an improved zero-noise extrapolation to effectively reduce adverse effects from inherent noise on current quantum devices.We showcase the utility of our quantum DFT+DMFT workflow by assessing the correlation effects on the electronic structure of a real material,Ca_(2)CuO_(2)Cl_(2),which is mapped to an effective single-band Hubbard Hamiltonian and the subsequently derived Anderson impurity model solved with up to 6 bath sites on available quantum hardware.Further,we carefully benchmark our quantum results with respect to exact reference solutions and experimental spectroscopy measurements.While challenges remain to scale our approach to larger,multi-orbital and multi-site systems with more bath sites,the present work marks an important milestone towards achieving utility-scale quantum computation in materials simulation.
