Optimizing the energy barrier of 2H-to-1T phase transformation plays a crucial role in modulating the intrinsic electronic structure of MoS_(2)to achieve satisfactory water-splitting performance,but remains a signific...Optimizing the energy barrier of 2H-to-1T phase transformation plays a crucial role in modulating the intrinsic electronic structure of MoS_(2)to achieve satisfactory water-splitting performance,but remains a significant challenge.Herein,we report a vacancy occupation-triggered phase transition strategy to fabricate a core-shell 1T phase nanorod structure,which is composed of S-vacancies decorated MoS_(2)as the core,and N,P co-doped carbons as the shell(1T-MoS_(2)@NPC).The co-insertion of N and P dopants into MoS_(2)can occupy partial S-vacancies,triggering a phase transformation from the semiconducting 2H phase to the conducting 1T phase with a reduced energy barrier.Profiting from the strong coupling effect between N,P dopants and S-vacancies,the as-made 1T-MoS_(2)@NPC exhibits excellent electrocatalytic activity for both HER(η_(10)=148 m V)and OER(η_(10)=232 mV)in alkaline solution.Meanwhile,a low cell voltage of 1.62 V is needed to drive a current density of 10mA cm^(-2)in 1.0 M KOH electrolyte.The theoretical calculation results reveal that the S-vacancies decorated C atoms in the meta-position relative to N,P atoms represent the most active HER and OER sites,which synergistically upshift the d band center and balance the rate-determining step,thus ensuring the simultaneous optimization of adsorption free energy and electronic structure.This vacancy-occupation-derived phase transformation strategy caused by non-metallic doping may provide valuable guidance for enhancing the performance of alkaline water electrolysis.展开更多
Charge-density-wave(CDW) materials with strongly correlated electrons have broadband light absorption and ultrafast response to light irradiation, and hence hold great potential in photodetection. 1 T-TaS2 is a typica...Charge-density-wave(CDW) materials with strongly correlated electrons have broadband light absorption and ultrafast response to light irradiation, and hence hold great potential in photodetection. 1 T-TaS2 is a typical CDW material with various thermodynamically CDW ground states at different temperatures and fertile out-of-equilibrium intermediate/hidden states. In particular, the light pulses can trigger melting of CDW ordering and also forms hidden states, which exhibits strikingly different electrical conductivity compared to the ground phase. Here, we review the recent research on phase transitions in 1 T-TaS2 and their potential applications in photodetection. We also discuss the ultrafast melting of CDW ordering by ultrafast laser irradiation and the out-of-equilibrium intermediate/hidden states by optical/electrical pulse. For photodetection, demonstrations of photoconductors and bolometers are introduced. Finally, we discuss some of the challenges that remain.展开更多
<span style="font-family:Verdana;">T</span><span style="font-family:Verdana;font-size:12px;">he T</span><span style="font-family:Verdana;font-size:12px;">i&l...<span style="font-family:Verdana;">T</span><span style="font-family:Verdana;font-size:12px;">he T</span><span style="font-family:Verdana;font-size:12px;">i</span><span style="font-family:Verdana;font-size:12px;">Se</span><sub><span style="font-family:Verdana;font-size:12px;">2</span></sub><span style="font-family:Verdana;font-size:12px;"> </span><span style="font-family:Verdana;font-size:12px;">nanosheets</span><span style="font-family:Verdana;font-size:12px;"> </span><span style="font-family:Verdana;font-size:12px;">were</span><span style="font-family:Verdana;font-size:12px;"> prepared by means of ultrasound-assisted liquid </span><span style="font-family:Verdana;font-size:12px;">phase exfoliation (LPE)</span><span style="font-family:Verdana;font-size:12px;"> and the </span><span style="font-family:Verdana;font-size:12px;">nonlinear </span><span style="font-family:Verdana;font-size:12px;">saturable absorption</span><span style="font-family:Verdana;font-size:12px;"> properties</span><span style="font-family:Verdana;font-size:12px;"> </span><span style="font-family:Verdana;font-size:12px;">were experimentally</span><span style="font-family:Verdana;font-size:12px;"> investigated. The modulation depth, saturation intensity and nonsaturable absorbance</span><span style="font-family:Verdana;font-size:12px;"> of the prepared </span><span style="font-family:Verdana;font-size:12px;">1T-TiSe</span><sub><span style="font-family:Verdana;font-size:12px;">2</span></sub><span style="font-family:Verdana;font-size:12px;"> </span><span style="font-family:Verdana;font-size:12px;">SA </span><span style="font-family:Verdana;font-size:12px;">were</span><span style="font-family:Verdana;font-size:12px;"> </span><span style="font-family:Verdana;font-size:12px;">1</span><span style="font-family:Verdana;font-size:12px;">5.7</span><span style="font-family:Verdana;font-size:12px;">%,</span><span style="font-family:Verdana;font-size:12px;"> 1.28 M</span><span style="font-family:Verdana;font-size:12px;">W/cm</span><sup><span style="font-family:Verdana;font-size:12px;vertical-align:super;">2</span></sup><span style="font-family:Verdana;font-size:12px;"> and 8.</span><span style="font-family:Verdana;font-size:12px;">2</span><span style="font-family:Verdana;font-size:12px;">%, </span><span style="font-family:Verdana;font-size:12px;">respectively</span><span style="font-family:Verdana;font-size:12px;">. Taking advantage of the saturable absorption properties of </span><span style="font-family:Verdana;font-size:12px;">T</span><span style="font-family:Verdana;font-size:12px;">i</span><span style="font-family:Verdana;font-size:12px;">Se</span><sub><span style="font-family:Verdana;font-size:12px;">2</span></sub><span style="font-family:Verdana;font-size:12px;">-based SA, a passively Q-switched erbium-doped fiber (EDF) laser was</span><span style="font-family:Verdana;font-size:12px;"> systematically demonstrated</span><span style="font-family:Verdana;font-size:12px;">. The pulse repetition rates varied from 24.50 kHz up to 73.79 kHz with the increasing pump power. The obtained shortest pulse width was 1.31 </span><span style="font-family:Verdana;font-size:12px;">μ</span><span style="font-family:Verdana;font-size:12px;">s with pulse energy of 79.28 nJ. The </span><span style="font-family:Verdana;font-size:12px;">system presented merits of low-cost SA preparation, system compactness,</span><span style="font-family:Verdana;font-size:12px;"> superb stability and high competition.</span>展开更多
基金supported by the National Natural Science Foundation of China(Grant No.22275210)the Natural Science Foundation of Shandong Province(Grant No.ZR2024QB025,ZR2023ME155)the Taishan Scholar Project of Shandong Province(tsqn202306226)。
文摘Optimizing the energy barrier of 2H-to-1T phase transformation plays a crucial role in modulating the intrinsic electronic structure of MoS_(2)to achieve satisfactory water-splitting performance,but remains a significant challenge.Herein,we report a vacancy occupation-triggered phase transition strategy to fabricate a core-shell 1T phase nanorod structure,which is composed of S-vacancies decorated MoS_(2)as the core,and N,P co-doped carbons as the shell(1T-MoS_(2)@NPC).The co-insertion of N and P dopants into MoS_(2)can occupy partial S-vacancies,triggering a phase transformation from the semiconducting 2H phase to the conducting 1T phase with a reduced energy barrier.Profiting from the strong coupling effect between N,P dopants and S-vacancies,the as-made 1T-MoS_(2)@NPC exhibits excellent electrocatalytic activity for both HER(η_(10)=148 m V)and OER(η_(10)=232 mV)in alkaline solution.Meanwhile,a low cell voltage of 1.62 V is needed to drive a current density of 10mA cm^(-2)in 1.0 M KOH electrolyte.The theoretical calculation results reveal that the S-vacancies decorated C atoms in the meta-position relative to N,P atoms represent the most active HER and OER sites,which synergistically upshift the d band center and balance the rate-determining step,thus ensuring the simultaneous optimization of adsorption free energy and electronic structure.This vacancy-occupation-derived phase transformation strategy caused by non-metallic doping may provide valuable guidance for enhancing the performance of alkaline water electrolysis.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.21673058 and 21822502)the Key Research Program of Frontier Sciences of Chinese Academy of Sciences(Grant No.QYZDB-SSW-SYS031)the Strategic Priority Research Program of Chinese Academy of Sciences(Grant No.XDB30000000)
文摘Charge-density-wave(CDW) materials with strongly correlated electrons have broadband light absorption and ultrafast response to light irradiation, and hence hold great potential in photodetection. 1 T-TaS2 is a typical CDW material with various thermodynamically CDW ground states at different temperatures and fertile out-of-equilibrium intermediate/hidden states. In particular, the light pulses can trigger melting of CDW ordering and also forms hidden states, which exhibits strikingly different electrical conductivity compared to the ground phase. Here, we review the recent research on phase transitions in 1 T-TaS2 and their potential applications in photodetection. We also discuss the ultrafast melting of CDW ordering by ultrafast laser irradiation and the out-of-equilibrium intermediate/hidden states by optical/electrical pulse. For photodetection, demonstrations of photoconductors and bolometers are introduced. Finally, we discuss some of the challenges that remain.
文摘<span style="font-family:Verdana;">T</span><span style="font-family:Verdana;font-size:12px;">he T</span><span style="font-family:Verdana;font-size:12px;">i</span><span style="font-family:Verdana;font-size:12px;">Se</span><sub><span style="font-family:Verdana;font-size:12px;">2</span></sub><span style="font-family:Verdana;font-size:12px;"> </span><span style="font-family:Verdana;font-size:12px;">nanosheets</span><span style="font-family:Verdana;font-size:12px;"> </span><span style="font-family:Verdana;font-size:12px;">were</span><span style="font-family:Verdana;font-size:12px;"> prepared by means of ultrasound-assisted liquid </span><span style="font-family:Verdana;font-size:12px;">phase exfoliation (LPE)</span><span style="font-family:Verdana;font-size:12px;"> and the </span><span style="font-family:Verdana;font-size:12px;">nonlinear </span><span style="font-family:Verdana;font-size:12px;">saturable absorption</span><span style="font-family:Verdana;font-size:12px;"> properties</span><span style="font-family:Verdana;font-size:12px;"> </span><span style="font-family:Verdana;font-size:12px;">were experimentally</span><span style="font-family:Verdana;font-size:12px;"> investigated. The modulation depth, saturation intensity and nonsaturable absorbance</span><span style="font-family:Verdana;font-size:12px;"> of the prepared </span><span style="font-family:Verdana;font-size:12px;">1T-TiSe</span><sub><span style="font-family:Verdana;font-size:12px;">2</span></sub><span style="font-family:Verdana;font-size:12px;"> </span><span style="font-family:Verdana;font-size:12px;">SA </span><span style="font-family:Verdana;font-size:12px;">were</span><span style="font-family:Verdana;font-size:12px;"> </span><span style="font-family:Verdana;font-size:12px;">1</span><span style="font-family:Verdana;font-size:12px;">5.7</span><span style="font-family:Verdana;font-size:12px;">%,</span><span style="font-family:Verdana;font-size:12px;"> 1.28 M</span><span style="font-family:Verdana;font-size:12px;">W/cm</span><sup><span style="font-family:Verdana;font-size:12px;vertical-align:super;">2</span></sup><span style="font-family:Verdana;font-size:12px;"> and 8.</span><span style="font-family:Verdana;font-size:12px;">2</span><span style="font-family:Verdana;font-size:12px;">%, </span><span style="font-family:Verdana;font-size:12px;">respectively</span><span style="font-family:Verdana;font-size:12px;">. Taking advantage of the saturable absorption properties of </span><span style="font-family:Verdana;font-size:12px;">T</span><span style="font-family:Verdana;font-size:12px;">i</span><span style="font-family:Verdana;font-size:12px;">Se</span><sub><span style="font-family:Verdana;font-size:12px;">2</span></sub><span style="font-family:Verdana;font-size:12px;">-based SA, a passively Q-switched erbium-doped fiber (EDF) laser was</span><span style="font-family:Verdana;font-size:12px;"> systematically demonstrated</span><span style="font-family:Verdana;font-size:12px;">. The pulse repetition rates varied from 24.50 kHz up to 73.79 kHz with the increasing pump power. The obtained shortest pulse width was 1.31 </span><span style="font-family:Verdana;font-size:12px;">μ</span><span style="font-family:Verdana;font-size:12px;">s with pulse energy of 79.28 nJ. The </span><span style="font-family:Verdana;font-size:12px;">system presented merits of low-cost SA preparation, system compactness,</span><span style="font-family:Verdana;font-size:12px;"> superb stability and high competition.</span>
