The experimental realization of observable phonon angular momentum(PAM)in feasible systems using relatively simple methods remains a critical challenge.Motivated by the chiral-induced spin selectivity effect,this stud...The experimental realization of observable phonon angular momentum(PAM)in feasible systems using relatively simple methods remains a critical challenge.Motivated by the chiral-induced spin selectivity effect,this study explores the generation of PAM during the transport of electrically driven polarons along a singlestranded helix structure.We demonstrate that the motion of a polaron under an applied electric field inherently induces a finite PAM,exhibiting drift-locked behavior between the PAM and the polaron.By analyzing the time evolution of PAM distribution at each site,we identify the observed PAM as a natural consequence of coherent superposition between lattice waves,in which the chiral structure selectively determines the direction of induced PAM.Furthermore,we examine the roles of two types of electron-phonon interactions and structural periodicity in modulating PAM.These findings highlight the potential of chiral molecules as platforms for PAM generation and offer new insights into developing phonon-spin-based devices for information processing and transmission.展开更多
The dynamic magnetic behavior of metal complexes correlates with their phonon modes,which depend on solid polymorphs.However,no systematic study has revealed the correlation between solid phases and spin-lattice relax...The dynamic magnetic behavior of metal complexes correlates with their phonon modes,which depend on solid polymorphs.However,no systematic study has revealed the correlation between solid phases and spin-lattice relaxation.Herein,we report the magnetism of a VO^(2+)-porphyrinato complex that contains dodecyl chains(1).Owing to the flexibility of the molecular structure,we successfully isolated the metastable crystalline phase 1m,the glass phase 1g and the stable crystalline phase 1s.Although the chemical compositions of the three phases are the same,1s with the lowest entropy exhibited the longest magnetic relaxation time.Our results suggest that(1)phase stabilization is an effective method for elongating the spin-lattice relaxation time and(2)spin-lattice relaxation correlates with the entropy of the solid.展开更多
The electrochemical CO_(2) reduction reaction(CO_(2)RR)to produce syngas offers a powerful strategy for achieving sustainable chemical production.Achieving syngas with tunable CO/H_(2) ratios within a wide potential w...The electrochemical CO_(2) reduction reaction(CO_(2)RR)to produce syngas offers a powerful strategy for achieving sustainable chemical production.Achieving syngas with tunable CO/H_(2) ratios within a wide potential window is highly desirable but challenging.Here,by doping Ga into Cu_(2)(OH)_(2)CO_(3) to engineer the interfacial hydrophobicity and electronic structure,we effectively controlled CO and H_(2) production during CO_(2) electroreduction.We tuned the CO/H_(2) ratio from 0.15 to 2.1,achieving a maximum 100% syngas production in a wide potential window(-0.6 to -1.8 V vs.RHE).Various characterization techniques,including in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy(ATR-SEIRAS)and in situ electrochemical impedance spectroscopy(EIS),revealed that appropriate Ga doping into Cu_(2)(OH)2CO_(3) facilitates CO_(2) mass transfer at the catalyst surface,thereby enhancing CO_(2)RR activity.In contrast,when the Ga doping ratio reaches 1.0,excessive surface hydrophobicity hinders CO_(2) reduction but facilitates the hydrogen evolution reaction(HER).Moreover,the Ga-induced modulation of the Cu+/Cu^(2+)ratio further exerts a synergistic effect on C^(2+)product selectivity.Additionally,as the Ga doping increases,the*CO binding configuration shifts from linearly bonded to bridge bonded,revealing the reaction pathway.This versatile control of the CO/H_(2) ratio in the CO_(2)RR offers significant opportunities for the direct transformation of CO_(2) into syngas.展开更多
The cold atom qubit platform emerges as an attractive choice for the next stage of quantum computation research,where a special family of synthetic analytical pulses has considerably improved the experimental performa...The cold atom qubit platform emerges as an attractive choice for the next stage of quantum computation research,where a special family of synthetic analytical pulses has considerably improved the experimental performance of Controlled-PHASE Rydberg blockade gates in recent studies.The success of Controlled-PHASE Rydberg blockade gates triggers the intriguing question of whether the two-qubit Rydberg blockade gate SWAP gate exists.Via investigating the transition linkage structure,we provide a definitive answer to this question and establish the method of fast SWAP Rydberg blockade gates with synthetic continuously modulated driving.These gate protocols use careful analysis to properly generate coherent population transfer and phase accumulation of the wave function in the atom-laser interaction process.They can adapt to finite Rydberg blockade strengths and bear considerable resistance to some major adverse effects such as laser fluctuations.Further examinations reveal that we can anticipate satisfying performances of the method with currently available experimental techniques in relevant research areas.展开更多
基金supported by the National Key R&D Project from Ministry of Science and Technology of China(Grant No.2022YFA1203100)the National Natural Science Foundation of China(Grant No.52350088)+1 种基金the Department of Science and Technology of Jiangsu Province(Grant No.BK20220032)the Postgraduate Research&Practice Innovation Program of Jiangsu Province(Grant No.KYCX241797)。
文摘The experimental realization of observable phonon angular momentum(PAM)in feasible systems using relatively simple methods remains a critical challenge.Motivated by the chiral-induced spin selectivity effect,this study explores the generation of PAM during the transport of electrically driven polarons along a singlestranded helix structure.We demonstrate that the motion of a polaron under an applied electric field inherently induces a finite PAM,exhibiting drift-locked behavior between the PAM and the polaron.By analyzing the time evolution of PAM distribution at each site,we identify the observed PAM as a natural consequence of coherent superposition between lattice waves,in which the chiral structure selectively determines the direction of induced PAM.Furthermore,we examine the roles of two types of electron-phonon interactions and structural periodicity in modulating PAM.These findings highlight the potential of chiral molecules as platforms for PAM generation and offer new insights into developing phonon-spin-based devices for information processing and transmission.
基金supported by the JSPS KAKENHI grants JP18K14242(Y.H.),JP19H05631(M.Y.),JP20K05540(T.Y.),JP20K15293(T.K.),and JP21K14645(Y.H.)the National Natural Science Foundation of China(NSFC,22150710513).P.M.Y.thanks for the support of the 111 Project(B18030)from ChinaThis work was performed under the approval of the Photon Factory Program Advisory Committee(Proposal No.2019G117,beamline 9A).
文摘The dynamic magnetic behavior of metal complexes correlates with their phonon modes,which depend on solid polymorphs.However,no systematic study has revealed the correlation between solid phases and spin-lattice relaxation.Herein,we report the magnetism of a VO^(2+)-porphyrinato complex that contains dodecyl chains(1).Owing to the flexibility of the molecular structure,we successfully isolated the metastable crystalline phase 1m,the glass phase 1g and the stable crystalline phase 1s.Although the chemical compositions of the three phases are the same,1s with the lowest entropy exhibited the longest magnetic relaxation time.Our results suggest that(1)phase stabilization is an effective method for elongating the spin-lattice relaxation time and(2)spin-lattice relaxation correlates with the entropy of the solid.
基金supported by the National Natural Science Foundation of China(22035002,22378192,and U22B20148)the Jiangsu Funding Program for Excellent Postdoctoral Talent(2024ZB272)+1 种基金the Postdoctoral Fellowship Program of China Postdoctoral Science Foundation(GZC20240701)the International Science and Technology Cooperation Project of Innovative Supporting Plan of Jiangsu Province(BZ2022040).
文摘The electrochemical CO_(2) reduction reaction(CO_(2)RR)to produce syngas offers a powerful strategy for achieving sustainable chemical production.Achieving syngas with tunable CO/H_(2) ratios within a wide potential window is highly desirable but challenging.Here,by doping Ga into Cu_(2)(OH)_(2)CO_(3) to engineer the interfacial hydrophobicity and electronic structure,we effectively controlled CO and H_(2) production during CO_(2) electroreduction.We tuned the CO/H_(2) ratio from 0.15 to 2.1,achieving a maximum 100% syngas production in a wide potential window(-0.6 to -1.8 V vs.RHE).Various characterization techniques,including in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy(ATR-SEIRAS)and in situ electrochemical impedance spectroscopy(EIS),revealed that appropriate Ga doping into Cu_(2)(OH)2CO_(3) facilitates CO_(2) mass transfer at the catalyst surface,thereby enhancing CO_(2)RR activity.In contrast,when the Ga doping ratio reaches 1.0,excessive surface hydrophobicity hinders CO_(2) reduction but facilitates the hydrogen evolution reaction(HER).Moreover,the Ga-induced modulation of the Cu+/Cu^(2+)ratio further exerts a synergistic effect on C^(2+)product selectivity.Additionally,as the Ga doping increases,the*CO binding configuration shifts from linearly bonded to bridge bonded,revealing the reaction pathway.This versatile control of the CO/H_(2) ratio in the CO_(2)RR offers significant opportunities for the direct transformation of CO_(2) into syngas.
基金Science and Technology Commission of Shanghai Municipality(24DP2600202)National Key Research and Development Program of China(2024YFB4504002)National Natural Science Foundation of China(92165107)。
文摘The cold atom qubit platform emerges as an attractive choice for the next stage of quantum computation research,where a special family of synthetic analytical pulses has considerably improved the experimental performance of Controlled-PHASE Rydberg blockade gates in recent studies.The success of Controlled-PHASE Rydberg blockade gates triggers the intriguing question of whether the two-qubit Rydberg blockade gate SWAP gate exists.Via investigating the transition linkage structure,we provide a definitive answer to this question and establish the method of fast SWAP Rydberg blockade gates with synthetic continuously modulated driving.These gate protocols use careful analysis to properly generate coherent population transfer and phase accumulation of the wave function in the atom-laser interaction process.They can adapt to finite Rydberg blockade strengths and bear considerable resistance to some major adverse effects such as laser fluctuations.Further examinations reveal that we can anticipate satisfying performances of the method with currently available experimental techniques in relevant research areas.
