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
Understanding the excited state dynamics of donor-acceptor(D-A)complexes is of fundamental importance both experimentally and theoretically.Herein,we have first explored the photoinduced dynamics of a recently synthes...Understanding the excited state dynamics of donor-acceptor(D-A)complexes is of fundamental importance both experimentally and theoretically.Herein,we have first explored the photoinduced dynamics of a recently synthesized paddle-wheel BODIPY-hexaoxatriphenylene(BODIPY is the abbreviation for BF_(2)-chelated dipyrromethenes)conjugates D-A complexes with the combination of both electronic structure calculations and nonadiabatic dynamics simulations.On the basis of computational results,we concluded that the BODIPY-hexaoxatriphenylene(BH)conjugates will be promoted to the local excited(LE)states of the BODIPY fragments upon excitation,which is followed by the ultrafast exciton transfer from LE state to charge transfer(CT).Instead of the photoinduced electron transfer process proposed in previous experimental work,such a exciton transfer process is accompanied with the photoinduced hole transfer from BODIPY to hexaoxatriphenylene.Additionally,solvent effects are found to play an important role in the photoinduced dynamics.Specifically,the hole transfer dynamics is accelerated by the acetonitrile solvent,which can be ascribed to significant influences of the solvents on the charge transfer states,i.e.the energy gaps between LE and CT excitons are reduced greatly and the non-adiabatic couplings are increased in the meantime.Our present work not only provides valuable insights into the underlying photoinduced mechanism of BH,but also can be helpful for the future design of novel donor-acceptor conjugates with better optoelectronic performance.展开更多
We report the thermal conductivities of monolayer （1L） and bilayer （2L） WS2 grown by chemical vapor deposition （CVD）, which are determined by use of temperature and excitation dependences of E2g^1 and A1g Raman ...We report the thermal conductivities of monolayer （1L） and bilayer （2L） WS2 grown by chemical vapor deposition （CVD）, which are determined by use of temperature and excitation dependences of E2g^1 and A1g Raman modes. The first-order temperature coefficients of E2g^1 and Alg modes in both supported and suspended WS2 layers were extracted. The frequency shift of the A3g mode with temperature is larger than that of the E1 mode for 1L-WS2, which is 2g attributed to stronger electron-phonon coupling for the A1g mode than that for the E12g mode. Moreover, by use of the shift of the phonon mode induced by laser heating, the thermal conductivities at room temperature were estimated to be 32 and 53 W/（m.K） for 1L- and 2L-WS2, respectively. Our results provide fundamental information about the thermal properties of WS2 layers, which is crucial for developing applications of atomically-thin WS2 devices.展开更多
In the light of the needs to develop high-performance heat transfer component for nation-level large-scale scientific projects of China,a hypervapotron experimental platform with supply of heat flux 1 10 MW m-2 was es...In the light of the needs to develop high-performance heat transfer component for nation-level large-scale scientific projects of China,a hypervapotron experimental platform with supply of heat flux 1 10 MW m-2 was established.With this platform,the multiphase flow and heat transfer phenomena on the surface of triangular fin when the subcooled water flowed through were observed and measured with the planar laser induced fluorescence(PLIF) and high-speed photography techniques.The temperature contour on the slice plane of fin symmetry was measured and the heat flux contour was processed based on gradient computation.It is confirmed that:1) PLIF with high-speed photography is very powerful technique to investigate the multiphase flow of hypervapotron quantitatively;2) evaporation is the primary way in heat transfer mechanism of hypervapotron flow under the condition of high heat flux.The techniques and results obtained will provide useful reference in the R&D of hypervapotron technology in China.展开更多
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 Natural Science Foundation of China(No.22003043 for Xiang-Yang Liu)the National Natural Science Foundation of China(No.21688102,No.21590801,and No.21520102005 for Ganglong Cui)+1 种基金Sichuan Science and Technology Program(No.2020YJ0161 for Xiang-Yang Liu)the High Performance Computing Center of Sichuan Normal University。
文摘Understanding the excited state dynamics of donor-acceptor(D-A)complexes is of fundamental importance both experimentally and theoretically.Herein,we have first explored the photoinduced dynamics of a recently synthesized paddle-wheel BODIPY-hexaoxatriphenylene(BODIPY is the abbreviation for BF_(2)-chelated dipyrromethenes)conjugates D-A complexes with the combination of both electronic structure calculations and nonadiabatic dynamics simulations.On the basis of computational results,we concluded that the BODIPY-hexaoxatriphenylene(BH)conjugates will be promoted to the local excited(LE)states of the BODIPY fragments upon excitation,which is followed by the ultrafast exciton transfer from LE state to charge transfer(CT).Instead of the photoinduced electron transfer process proposed in previous experimental work,such a exciton transfer process is accompanied with the photoinduced hole transfer from BODIPY to hexaoxatriphenylene.Additionally,solvent effects are found to play an important role in the photoinduced dynamics.Specifically,the hole transfer dynamics is accelerated by the acetonitrile solvent,which can be ascribed to significant influences of the solvents on the charge transfer states,i.e.the energy gaps between LE and CT excitons are reduced greatly and the non-adiabatic couplings are increased in the meantime.Our present work not only provides valuable insights into the underlying photoinduced mechanism of BH,but also can be helpful for the future design of novel donor-acceptor conjugates with better optoelectronic performance.
文摘We report the thermal conductivities of monolayer （1L） and bilayer （2L） WS2 grown by chemical vapor deposition （CVD）, which are determined by use of temperature and excitation dependences of E2g^1 and A1g Raman modes. The first-order temperature coefficients of E2g^1 and Alg modes in both supported and suspended WS2 layers were extracted. The frequency shift of the A3g mode with temperature is larger than that of the E1 mode for 1L-WS2, which is 2g attributed to stronger electron-phonon coupling for the A1g mode than that for the E12g mode. Moreover, by use of the shift of the phonon mode induced by laser heating, the thermal conductivities at room temperature were estimated to be 32 and 53 W/（m.K） for 1L- and 2L-WS2, respectively. Our results provide fundamental information about the thermal properties of WS2 layers, which is crucial for developing applications of atomically-thin WS2 devices.
基金supported by the Fundamental Research Funds for the Central Universities of Chinathe National Magnetic Confined Fusion Energy Program of China (Grant No. 2009GB104005)
文摘In the light of the needs to develop high-performance heat transfer component for nation-level large-scale scientific projects of China,a hypervapotron experimental platform with supply of heat flux 1 10 MW m-2 was established.With this platform,the multiphase flow and heat transfer phenomena on the surface of triangular fin when the subcooled water flowed through were observed and measured with the planar laser induced fluorescence(PLIF) and high-speed photography techniques.The temperature contour on the slice plane of fin symmetry was measured and the heat flux contour was processed based on gradient computation.It is confirmed that:1) PLIF with high-speed photography is very powerful technique to investigate the multiphase flow of hypervapotron quantitatively;2) evaporation is the primary way in heat transfer mechanism of hypervapotron flow under the condition of high heat flux.The techniques and results obtained will provide useful reference in the R&D of hypervapotron technology in China.
