Although photonics presents the fastest and most energy-efficient method of data transfer,magnetism still offers the cheapest and most natural way to store data.The ultrafast and energy-efficient optical control of ma...Although photonics presents the fastest and most energy-efficient method of data transfer,magnetism still offers the cheapest and most natural way to store data.The ultrafast and energy-efficient optical control of magnetism is presently a missing technological link that prevents us from reaching the next evolution in information processing.The discovery of all-optical magnetization reversal in GdFeCo with the help of 100fs laser pulses has further aroused intense interest in this compelling problem.Although the applicability of this approach to high-speed data processing depends vitally on the maximum repetition rate of the switching,the latter remains virtually unknown.Here we experimentally unveil the ultimate frequency of repetitive all-optical magnetization reversal through time-resolved studies of the dual-shot magnetization dynamics in Gd27 Fe63.87 C09.T3.Varying the intensities of the shots and the shotto-shot separation,we reveal the conditions for ultrafast writing and the fastest possible restoration of magnetic bits.It is shown that although magnetic writing launched by the first shot is completed after 100 ps,a reliable rewriting of the bit by the second shot requires separating the shots by at least 300 ps.Using two shots partially overlapping in space and minimally separated by 300 ps,we demonstrate an approach for GHz magnetic writing that can be scaled down to sizes below the diffraction limit.展开更多
Auranofin(AF)is the most used gold(I)-containing drug,whose mechanism of action involves targeting sulfur and selenium-containing amino acids,including cysteine(Cys)and selenocysteine(Sec).These residues are present i...Auranofin(AF)is the most used gold(I)-containing drug,whose mechanism of action involves targeting sulfur and selenium-containing amino acids,including cysteine(Cys)and selenocysteine(Sec).These residues are present in the active sites of crucial proteins including thioredoxin reductase.Despite extensive exploration of AF-protein interactions over the years,experimental data at the molecular level are still limited.In this work,we studied the vibrational and structural features of solvent-free complexes obtained by the reaction of AF with Cys and Sec,[(Et_(3)P)AuCys]^(+) and[(Et_(3)P)AuSec]^(+) ions,respectively.Using tandem mass spectrometry and IR ion spectroscopy supported by density functional theory(DFT)calculations,we unveiled markedly different behaviors for the Cys and Sec bound complexes.In particular,our results indicate that,whereas the[(Et_(3)P)AuSec]^(+) ions are mainly Se-bound,in agreement with the well-known affinity of Se for gold(I),the sampled[(Et_(3)P)AuCys]^(+) ionic population is composed of both N-and S-bound isomers,with their ratio depending on the dielectric constant of the solvent used in the starting solution.Additionally,we found that the deamination process occurring in the gas-phase during collision-induced dissociation experiments significantly differ between the two complexes.This work's findings contribute to a deeper understanding of AF's reactivity with Cys and Sec-containing protein targets and highlight how the chemical environment may influence target selectivity of gold-containing drugs,which is crucial for their pharmacological activities.展开更多
基金We are grateful to Dr.Dmytro V.Afanasiev,Tonnie Toonen,Dr.Bowen Jiang,and Dr.Sergey Semin for their professional technical support This research is financially supported by the National Key R&D Program of China(2018YFB1107200)Ministry of Science and Technology of the Peopled Republic of China(MOST)(Grant numbers 2016丫FA0300802 and 2018YFE0109200)+6 种基金National Natural Science Foundation of China(NSFC)(61975066 and 11604123)Guangdong Basic and Applied Basic Research Foundation(2019A1515010864)Fundamental Research Funds for the Central Universities(21620413)Guangdong Provincial Innovation and Entrepreneurship Project(Grant 2016ZT06D081)Grant-in-Aid for Scientific Research on Innovative Area,Nano Spin Conversion Science1(Grant number 26103005)‘Nano Spin Conversion Science'(Grant number 26103004)European Research Council ERC,Grant agreement number 339813(Exchange),and Netherlands Organization for Scientific Research(NWO).
文摘Although photonics presents the fastest and most energy-efficient method of data transfer,magnetism still offers the cheapest and most natural way to store data.The ultrafast and energy-efficient optical control of magnetism is presently a missing technological link that prevents us from reaching the next evolution in information processing.The discovery of all-optical magnetization reversal in GdFeCo with the help of 100fs laser pulses has further aroused intense interest in this compelling problem.Although the applicability of this approach to high-speed data processing depends vitally on the maximum repetition rate of the switching,the latter remains virtually unknown.Here we experimentally unveil the ultimate frequency of repetitive all-optical magnetization reversal through time-resolved studies of the dual-shot magnetization dynamics in Gd27 Fe63.87 C09.T3.Varying the intensities of the shots and the shotto-shot separation,we reveal the conditions for ultrafast writing and the fastest possible restoration of magnetic bits.It is shown that although magnetic writing launched by the first shot is completed after 100 ps,a reliable rewriting of the bit by the second shot requires separating the shots by at least 300 ps.Using two shots partially overlapping in space and minimally separated by 300 ps,we demonstrate an approach for GHz magnetic writing that can be scaled down to sizes below the diffraction limit.
基金funded by Sapienza Universitàdi RomaProgetti medi di Ateneo 2023,grant number RM123188F7509A0Bfrom LASERLAB-EUROPE(grant agreement No.871124,European Union’s Horizon 2020 research and innovation programme)+2 种基金the Nederlandse Organisatie voor Wetenschappelijk Onderzoek(NWO)for the support of the FELIX Laboratorythe CINECA award,under the ISCRA initiative,for the availability of high-performance computing resources and support(project IsCb5_G4MeFMO)support funded by the European Union NextGenerationEU,under the National Recovery and Resilience Plan(NRRP),Mission 4 Component 2 M4C2,Investment 1.5 Call for tender No.3277 of 30.12.2021,Italian Ministry of University,Award Number:ECS00000041,Project Title:“Innovation,digitalization and sustainability for the diffused economy in Central Italy”,Concession Degree No.1057 of 23.06.2022 adopted by the Italian Ministry of University.CUP:D73C22000840006.
文摘Auranofin(AF)is the most used gold(I)-containing drug,whose mechanism of action involves targeting sulfur and selenium-containing amino acids,including cysteine(Cys)and selenocysteine(Sec).These residues are present in the active sites of crucial proteins including thioredoxin reductase.Despite extensive exploration of AF-protein interactions over the years,experimental data at the molecular level are still limited.In this work,we studied the vibrational and structural features of solvent-free complexes obtained by the reaction of AF with Cys and Sec,[(Et_(3)P)AuCys]^(+) and[(Et_(3)P)AuSec]^(+) ions,respectively.Using tandem mass spectrometry and IR ion spectroscopy supported by density functional theory(DFT)calculations,we unveiled markedly different behaviors for the Cys and Sec bound complexes.In particular,our results indicate that,whereas the[(Et_(3)P)AuSec]^(+) ions are mainly Se-bound,in agreement with the well-known affinity of Se for gold(I),the sampled[(Et_(3)P)AuCys]^(+) ionic population is composed of both N-and S-bound isomers,with their ratio depending on the dielectric constant of the solvent used in the starting solution.Additionally,we found that the deamination process occurring in the gas-phase during collision-induced dissociation experiments significantly differ between the two complexes.This work's findings contribute to a deeper understanding of AF's reactivity with Cys and Sec-containing protein targets and highlight how the chemical environment may influence target selectivity of gold-containing drugs,which is crucial for their pharmacological activities.
