Comprehension of photon-triggered molecular processes is essential in the study of various important topics in physics,chemistry,and biology.Here we propose a correlated tunneling picture to understand the dissociativ...Comprehension of photon-triggered molecular processes is essential in the study of various important topics in physics,chemistry,and biology.Here we propose a correlated tunneling picture to understand the dissociative ionization process of molecules in intense laser fields based on a quantum model developed in the framework of many-body S-matrix theory including nuclear vibrational motion.In this quantum correlation picture,the single ionization of H_(2)and the subsequent electron-ion recollisioninduced dissociation are considered as an entangled correlated process.It enables us to attribute the interference pattern in the joint-energy spectra to combined effects of single-slit diffraction and multi-slit interference of correlated electron-nuclear wave packets in the time domain.Our work opens a new avenue to understanding molecular dissociative ionization processes in external fields.展开更多
Multiphoton resonant excitation and frustrated tunneling ionization,manifesting the photonic and optical nature of the driving light via direct excitation and electron recapture,respectively,are complementary mechanis...Multiphoton resonant excitation and frustrated tunneling ionization,manifesting the photonic and optical nature of the driving light via direct excitation and electron recapture,respectively,are complementary mechanisms to access Rydberg state excitation(RSE)of atoms and molecules in an intense laser field.However,clear identification and manipulation of their individual contributions in the light-induced RSE process remain experimentally challenging.Here,we bridge this gap by exploring the dissociative and nondissociative RSE of H2 molecules using bicircular two-color laser pulses.Depending on the relative field strength and polarization helicity of the two colors,the RSE probability can be boosted by more than one order of magnitude by exploiting the laser waveform-dependent field effect.The role of the photon effect is readily strengthened with increasing relative strength of the second-harmonic field of the two colors regardless of the polarization helicity.As compared to the nondissociative RSE forming H2,the field effect in producing the dissociative RSE channel of eHt;HT is moderately suppressed,which is primarily accessed via a three-step sequential process separated by molecular bond stretching.Our work paves the way toward a comprehensive understanding of the interplay of the underlying field and photon effects in the strong-field RSE process,as well as facilitating the generation of Rydberg states optimized with tailored characteristics.展开更多
基金supported by the National Key Research and Development Program of China(Grant No.2019YFA0307700)the National Natural Science Foundation of China(Grant Nos.12274273,12304379,11925405+2 种基金12304304)the Innovation Program for Quantum Science and Technology(Grant No.2021ZD0302101)the Natural and Science Foundation of Top Talent of SZTU(Grant No.GDRC202202)。
文摘Comprehension of photon-triggered molecular processes is essential in the study of various important topics in physics,chemistry,and biology.Here we propose a correlated tunneling picture to understand the dissociative ionization process of molecules in intense laser fields based on a quantum model developed in the framework of many-body S-matrix theory including nuclear vibrational motion.In this quantum correlation picture,the single ionization of H_(2)and the subsequent electron-ion recollisioninduced dissociation are considered as an entangled correlated process.It enables us to attribute the interference pattern in the joint-energy spectra to combined effects of single-slit diffraction and multi-slit interference of correlated electron-nuclear wave packets in the time domain.Our work opens a new avenue to understanding molecular dissociative ionization processes in external fields.
基金the National Key R&D Program of China(Grant No.2018YFA0306303)the National Natural Science Foundation of China(Grant Nos.11834004,61690224,92150105,11904103,12241407,and 12227807)the Science and Technology Commission of Shanghai Municipality(Grant No.21ZR1420100).
文摘Multiphoton resonant excitation and frustrated tunneling ionization,manifesting the photonic and optical nature of the driving light via direct excitation and electron recapture,respectively,are complementary mechanisms to access Rydberg state excitation(RSE)of atoms and molecules in an intense laser field.However,clear identification and manipulation of their individual contributions in the light-induced RSE process remain experimentally challenging.Here,we bridge this gap by exploring the dissociative and nondissociative RSE of H2 molecules using bicircular two-color laser pulses.Depending on the relative field strength and polarization helicity of the two colors,the RSE probability can be boosted by more than one order of magnitude by exploiting the laser waveform-dependent field effect.The role of the photon effect is readily strengthened with increasing relative strength of the second-harmonic field of the two colors regardless of the polarization helicity.As compared to the nondissociative RSE forming H2,the field effect in producing the dissociative RSE channel of eHt;HT is moderately suppressed,which is primarily accessed via a three-step sequential process separated by molecular bond stretching.Our work paves the way toward a comprehensive understanding of the interplay of the underlying field and photon effects in the strong-field RSE process,as well as facilitating the generation of Rydberg states optimized with tailored characteristics.
