激发态能量转移(Excitation Energy Transfer,EET)作为一类重要的光物理现象,被广泛用于比率型荧光探针和分子灯标的设计以及DNA检测等多个领域.影响EET效率的两个重要因素是供受体间的空间距离和光谱交盖,通过调节供受体间的空间距离...激发态能量转移(Excitation Energy Transfer,EET)作为一类重要的光物理现象,被广泛用于比率型荧光探针和分子灯标的设计以及DNA检测等多个领域.影响EET效率的两个重要因素是供受体间的空间距离和光谱交盖,通过调节供受体间的空间距离或光谱重叠程度来调控能量转移过程,实现对目标客体的双波长比率检测.综述了基于不同供受体荧光团的EET体系、供受体间的连接方式对能量转移效率的影响,以及通过调控供受体间光谱重叠程度或空间距离,获得识别不同客体的比率型荧光探针,并对EET机理的比率型荧光探针的设计以及未来在生物成像和医学检测等领域的应用进行了展望.展开更多
Triplet-triplet energy transfer in fluorene dimer with electronic structure calculations. The two is investigated by combining rate theories key parameters for the control of energy transfer, electronic coupling and r...Triplet-triplet energy transfer in fluorene dimer with electronic structure calculations. The two is investigated by combining rate theories key parameters for the control of energy transfer, electronic coupling and reorganization energy, are calculated based on the diabatic states constructed by the constrained density functional theory. The fluctuation of the electronic coupling is further revealed by molecular dynamics simulation. Succeedingly, the diagonal and off-diagonal fluctuations of the Hamiltonian are mapped from the correlation functions of those parameters, and the rate is then estimated both from the perturbation theory and wavepacket diffusion method. The results manifest that both the static and dynamic fluctuations enhance the rate significantly, but the rate from the dynamic fluctuation is smaller than that from the static fluctuation.展开更多
In this work,we employ electronic structure calculations and nonadiabatic dynamics simulations based on many-body Green function and BetheSalpeter equation(GW/BSE)methods to study excited-state properties of a zinc ph...In this work,we employ electronic structure calculations and nonadiabatic dynamics simulations based on many-body Green function and BetheSalpeter equation(GW/BSE)methods to study excited-state properties of a zinc phthalocyanine-fullerene(ZnPcC_(60))dyad with 6-6 and 5-6 configurations.In the former,the initially populated locally excited(LE)state of ZnPc is the lowest S1 state and thus,its subsequent charge separation is relatively slow.In contrast,in the latter,the S1 state is the LE state of C_(60)while the LE state of ZnPc is much higher in energy.There also exist several charge-transfer(CT)states between the LE states of ZnPc and C_(60).Thus,one can see apparent charge separation dynamics during excited-state relaxation dynamics from the LE state of ZnPc to that of C_(60).These points are verified in dynamics simulations.In the first 200 fs,there is a rapid excitation energy transfer from ZnPc to C_(60),followed by an ultrafast charge separation to form a CT intermediate state.This process is mainly driven by hole transfer from C_(60)to ZnPc.The present work demonstrates that different bonding patterns(i.e.5-6 and 6-6)of the C−N linker can be used to tune excited-state properties and thereto optoelectronic properties of covalently bonded ZnPc-C_(60)dyads.Methodologically,it is proven that combined GW/BSE nonadiabatic dynamics method is a practical and reliable tool for exploring photoinduced dynamics of nonperiodic dyads,organometallic molecules,quantum dots,nanoclusters,etc.展开更多
A transfer-reaction experiment of ~9Be(~9Be,^(10)Be)~8Be was performed at a beam energy of 45 Me V.Excited states in ^(10)Be up to 18.80 Me V are produced using missing mass and invariant mass methods.Most of the obse...A transfer-reaction experiment of ~9Be(~9Be,^(10)Be)~8Be was performed at a beam energy of 45 Me V.Excited states in ^(10)Be up to 18.80 Me V are produced using missing mass and invariant mass methods.Most of the observed high-lying resonant states,reconstructed from theα+~6He and t+~7Li decay channels,agree with the previously reported results.In addition,two new resonances at 15.6 and 18.8 Me V are identified from the present measurement.The 18.55 Me V state is found to decay into both the t + ~7Lig:s: and t + ~7Li?(0.478 MeV) channels, with a relative branching ratio of 0:93 ± 0:33. Further theoretical investigations are encouraged to interpret this new information on cluster structure in neutron-rich light nuclei.展开更多
文摘激发态能量转移(Excitation Energy Transfer,EET)作为一类重要的光物理现象,被广泛用于比率型荧光探针和分子灯标的设计以及DNA检测等多个领域.影响EET效率的两个重要因素是供受体间的空间距离和光谱交盖,通过调节供受体间的空间距离或光谱重叠程度来调控能量转移过程,实现对目标客体的双波长比率检测.综述了基于不同供受体荧光团的EET体系、供受体间的连接方式对能量转移效率的影响,以及通过调控供受体间光谱重叠程度或空间距离,获得识别不同客体的比率型荧光探针,并对EET机理的比率型荧光探针的设计以及未来在生物成像和医学检测等领域的应用进行了展望.
基金This work was supported by the National Natural Science Foundation of China （No.20833004 and No.21073146） and the Research Fund for the Doctoral Program of Higher Education of China （No.200803840009）.
文摘Triplet-triplet energy transfer in fluorene dimer with electronic structure calculations. The two is investigated by combining rate theories key parameters for the control of energy transfer, electronic coupling and reorganization energy, are calculated based on the diabatic states constructed by the constrained density functional theory. The fluctuation of the electronic coupling is further revealed by molecular dynamics simulation. Succeedingly, the diagonal and off-diagonal fluctuations of the Hamiltonian are mapped from the correlation functions of those parameters, and the rate is then estimated both from the perturbation theory and wavepacket diffusion method. The results manifest that both the static and dynamic fluctuations enhance the rate significantly, but the rate from the dynamic fluctuation is smaller than that from the static fluctuation.
基金support from the National Natural Science Foundation of China(No.21688102,No.21590801,and No.21520102005)support from Sichuan Science and Technology Program Grant(2020YJ0161)。
文摘In this work,we employ electronic structure calculations and nonadiabatic dynamics simulations based on many-body Green function and BetheSalpeter equation(GW/BSE)methods to study excited-state properties of a zinc phthalocyanine-fullerene(ZnPcC_(60))dyad with 6-6 and 5-6 configurations.In the former,the initially populated locally excited(LE)state of ZnPc is the lowest S1 state and thus,its subsequent charge separation is relatively slow.In contrast,in the latter,the S1 state is the LE state of C_(60)while the LE state of ZnPc is much higher in energy.There also exist several charge-transfer(CT)states between the LE states of ZnPc and C_(60).Thus,one can see apparent charge separation dynamics during excited-state relaxation dynamics from the LE state of ZnPc to that of C_(60).These points are verified in dynamics simulations.In the first 200 fs,there is a rapid excitation energy transfer from ZnPc to C_(60),followed by an ultrafast charge separation to form a CT intermediate state.This process is mainly driven by hole transfer from C_(60)to ZnPc.The present work demonstrates that different bonding patterns(i.e.5-6 and 6-6)of the C−N linker can be used to tune excited-state properties and thereto optoelectronic properties of covalently bonded ZnPc-C_(60)dyads.Methodologically,it is proven that combined GW/BSE nonadiabatic dynamics method is a practical and reliable tool for exploring photoinduced dynamics of nonperiodic dyads,organometallic molecules,quantum dots,nanoclusters,etc.
基金supported by the National Basic Research Program of China (Grant No. 2013CB834402)the National Natural Science Foundation of China (Grant Nos. 11535004, 11275011, 11375017, and 11275001)
文摘A transfer-reaction experiment of ~9Be(~9Be,^(10)Be)~8Be was performed at a beam energy of 45 Me V.Excited states in ^(10)Be up to 18.80 Me V are produced using missing mass and invariant mass methods.Most of the observed high-lying resonant states,reconstructed from theα+~6He and t+~7Li decay channels,agree with the previously reported results.In addition,two new resonances at 15.6 and 18.8 Me V are identified from the present measurement.The 18.55 Me V state is found to decay into both the t + ~7Lig:s: and t + ~7Li?(0.478 MeV) channels, with a relative branching ratio of 0:93 ± 0:33. Further theoretical investigations are encouraged to interpret this new information on cluster structure in neutron-rich light nuclei.
