Rabi oscillations in a stretching molecule

Shengzhe Pan; Chenxi Hu; Wenbin Zhang; Zhaohan Zhang; Lianrong Zhou; Chenxu Lu; Peifen Lu; Hongcheng Ni; Jian Wu; Feng He

doi:10.1038/s41377-023-01075-9

Go to Nature Website

Your Location：

Home >

Browse articles >

Rabi oscillations in a stretching molecule

Original Articles

- Rabi oscillations in a stretching molecule
- Rabi oscillations in a stretching molecule
- 光：科学与应用 2023年12卷第2期页码：239-247
- Affiliations：
  
  1.State Key Laboratory of Precision Spectroscopy, East China Normal University, Shanghai, 200241, China
  2.Key Laboratory for Laser Plasmas (Ministry of Education) and School of Physics and Astronomy, Collaborative Innovation Center of IFSA (CICIFSA), Shanghai Jiao Tong University, Shanghai, 200240, China
  3.Collaborative Innovation Center of Extreme Optics, Shanxi University, Taiyuan, Shanxi, 030006, China
  4.Chongqing Key Laboratory of Precision Optics, Chongqing Institute of East China Normal University, Chongqing, 401121, China
  5.CAS Center for Excellence in Ultra-intense Laser Science, Shanghai, 201800, China
- Author bio：
  
  Jian Wu (jwu@phy.ecnu.edu.cn)
  Jian Wu (jwu@phy.ecnu.edu.cn)
- Funds：
- DOI：10.1038/s41377-023-01075-9
  中图分类号：
- 纸质出版日期：2023-2-28，
  
  网络出版日期：2023-2-2，
  
  收稿日期：2022-6-16，
  
  修回日期：2023-1-7，
  
  录用日期：2023-1-9
Scan for full text
Rabi oscillations in a stretching molecule[J]. 光：科学与应用, 2023,12(2):239-247.

Pan, S. Z. et al. Rabi oscillations in a stretching molecule. Light: Science & Applications, 12, 239-247 (2023).
Rabi oscillations in a stretching molecule[J]. 光：科学与应用, 2023,12(2):239-247. DOI： 10.1038/s41377-023-01075-9.

Pan, S. Z. et al. Rabi oscillations in a stretching molecule. Light: Science & Applications, 12, 239-247 (2023). DOI： 10.1038/s41377-023-01075-9.

摘要

Abstract

Rabi oscillation is an elementary laser-driven physical process in atoms and artificial atoms from solid-state systems

while it is rarely demonstrated in molecules. Here

we investigate the bond-length-dependent Rabi oscillations with varying Rabi frequencies in strong-laser-field dissociation of H

. The coupling of the bond stretching and Rabi oscillations makes the nuclei gain different kinetic energies while the electron is alternatively absorbing and emitting photons. The resulting proton kinetic energy spectra show rich structures beyond the prediction of the Floquet theorem and the well-accepted resonant one-photon dissociation pathway. Our study shows that the laser-driven Rabi oscillations accompanied by nuclear motions are essential to understanding the bond-breaking mechanism and provide a time-resolved perspective to manipulate rich dynamics of the strong-laser-field dissociation of molecules.

关键词

Keywords

references

I. I. Rabi . On the process of space quantization . Phys. Rev. , 1936 . 49 324 -328 . DOI:10.1103/PhysRev.49.324http://doi.org/10.1103/PhysRev.49.324 .

T. H. Stievater , 等 . Rabi oscillations of excitons in single quantum dots . Phys. Rev. Lett. , 2001 . 87 133603 DOI:10.1103/PhysRevLett.87.133603http://doi.org/10.1103/PhysRevLett.87.133603 .

T. Yoshie , 等 . Vacuum Rabi splitting with a single quantum dot in a photonic crystal nanocavity . Nature , 2004 . 432 200 -203 . DOI:10.1038/nature03119http://doi.org/10.1038/nature03119 .

D. Press , 等 . Complete quantum control of a single quantum dot spin using ultrafast optical pulses . Nature , 2008 . 456 218 -221 . DOI:10.1038/nature07530http://doi.org/10.1038/nature07530 .

A. Blais , 等 . Cavity quantum electrodynamics for superconducting electrical circuits: an architecture for quantum computation . Phys. Rev. A , 2004 . 69 062320 DOI:10.1103/PhysRevA.69.062320http://doi.org/10.1103/PhysRevA.69.062320 .

A. Feist , 等 . Quantum coherent optical phase modulation in an ultrafast transmission electron microscope . Nature , 2015 . 521 200 -203 . DOI:10.1038/nature14463http://doi.org/10.1038/nature14463 .

E. Pedrozo-Peñafiel , 等 . Entanglement on an optical atomic-clock transition . Nature , 2020 . 588 414 -418 . DOI:10.1038/s41586-020-3006-1http://doi.org/10.1038/s41586-020-3006-1 .

M. D. Lukin , 等 . Dipole blockade and quantum information processing in mesoscopic atomic ensembles . Phys. Rev. Lett. , 2001 . 87 037901 DOI:10.1103/PhysRevLett.87.037901http://doi.org/10.1103/PhysRevLett.87.037901 .

Y. O. Dudin , 等 . Observation of coherent many-body Rabi oscillations . Nat. Phys. , 2012 . 8 790 -794 . DOI:10.1038/nphys2413http://doi.org/10.1038/nphys2413 .

Z. G. Sun , N. Lou . Autler-Townes splitting in the multiphoton resonance ionization spectrum of molecules produced by ultrashort laser pulses . Phys. Rev. Lett. , 2003 . 91 023002 DOI:10.1103/PhysRevLett.91.023002http://doi.org/10.1103/PhysRevLett.91.023002 .

A. Palacios , H. Bachau , F. Martín . Step-ladder Rabi oscillations in molecules exposed to intense ultrashort vuv pulses . Phys. Rev. A , 2006 . 74 031402 DOI:10.1103/PhysRevA.74.031402http://doi.org/10.1103/PhysRevA.74.031402 .

S. H. Autler , C. H. Townes . Stark effect in rapidly varying fields . Phys. Rev. , 1955 . 100 703 -722 . DOI:10.1103/PhysRev.100.703http://doi.org/10.1103/PhysRev.100.703 .

R. R. Freeman , 等 . Above-threshold ionization with subpicosecond laser pulses . Phys. Rev. Lett. , 1987 . 59 1092 -1095 . DOI:10.1103/PhysRevLett.59.1092http://doi.org/10.1103/PhysRevLett.59.1092 .

M. Fushitani , 等 . Femtosecond two-photon Rabi oscillations in excited He driven by ultrashort intense laser fields . Nat. Photonics , 2016 . 10 102 -105 . DOI:10.1038/nphoton.2015.228http://doi.org/10.1038/nphoton.2015.228 .

V. Stooß , 等 . Real-time reconstruction of the strong-field-driven dipole response . Phys. Rev. Lett. , 2018 . 121 173005 DOI:10.1103/PhysRevLett.121.173005http://doi.org/10.1103/PhysRevLett.121.173005 .

S. Hughes . Breakdown of the area theorem: carrier-wave Rabi flopping of femtosecond optical pulses . Phys. Rev. Lett. , 1998 . 81 3363 -3366 . DOI:10.1103/PhysRevLett.81.3363http://doi.org/10.1103/PhysRevLett.81.3363 .

M. F. Ciappina , 等 . Carrier-wave Rabi-flopping signatures in high-order harmonic generation for alkali atoms . Phys. Rev. Lett. , 2015 . 114 143902 DOI:10.1103/PhysRevLett.114.143902http://doi.org/10.1103/PhysRevLett.114.143902 .

A. F. Linskens , 等 . Two-photon Rabi oscillations . Phys. Rev. A , 1996 . 54 4854 -4862 . DOI:10.1103/PhysRevA.54.4854http://doi.org/10.1103/PhysRevA.54.4854 .

S. Magnier , M. Persico , N. Rahman . Rabi oscillations between dissociative molecular states . Phys. Rev. Lett. , 1999 . 83 2159 -2162 . DOI:10.1103/PhysRevLett.83.2159http://doi.org/10.1103/PhysRevLett.83.2159 .

C. X. Hu , 等 . Angle-resolved Rabi flopping in strong-field dissociation of molecules . Phys. Rev. A , 2021 . 103 043122 DOI:10.1103/PhysRevA.103.043122http://doi.org/10.1103/PhysRevA.103.043122 .

A. K. Gupta , D. Neuhauser . Rabi-oscillations-induced multiharmonic emission in a Maxwell-Schrödinger study of a dense sample of molecules . Int. J. Quantum Chem. , 2001 . 81 260 -267 . DOI:10.1002/1097-461X(2001)81:4<260::AID-QUA3>3.0.CO;2-Mhttp://doi.org/10.1002/1097-461X(2001)81:4<260::AID-QUA3>3.0.CO;2-M .

P. H. Bucksbaum , 等 . Softening of the H2+ molecular bond in intense laser fields . Phys. Rev. Lett. , 1990 . 64 1883 -1886 . DOI:10.1103/PhysRevLett.64.1883http://doi.org/10.1103/PhysRevLett.64.1883 .

T. Ergler , 等 . Time-resolved imaging and manipulation of H2 fragmentation in intense laser fields . Phys. Rev. Lett. , 2005 . 95 093001 DOI:10.1103/PhysRevLett.95.093001http://doi.org/10.1103/PhysRevLett.95.093001 .

J. McKenna , 等 . Enhancing high-order above-threshold dissociation of H2+ beams with few-cycle laser pulses . Phys. Rev. Lett. , 2008 . 100 133001 DOI:10.1103/PhysRevLett.100.133001http://doi.org/10.1103/PhysRevLett.100.133001 .

A. Staudte , 等 . Angular tunneling ionization probability of fixed-in-space H2 molecules in intense laser pulses . Phys. Rev. Lett. , 2009 . 102 033004 DOI:10.1103/PhysRevLett.102.033004http://doi.org/10.1103/PhysRevLett.102.033004 .

J. McKenna , 等 . Suppressed dissociation of H2+ vibrational states by reduced dipole coupling . Phys. Rev. Lett. , 2009 . 103 103006 DOI:10.1103/PhysRevLett.103.103006http://doi.org/10.1103/PhysRevLett.103.103006 .

J. Wu , 等 . Understanding the role of phase in chemical bond breaking with coincidence angular streaking . Nat. Commun. , 2013 . 4 2177 DOI:10.1038/ncomms3177http://doi.org/10.1038/ncomms3177 .

H. Xu , 等 . Coherent control of the dissociation probability of H2+ in ω-3ω two-color field . Phys. Rev. A , 2016 . 93 063416 DOI:10.1103/PhysRevA.93.063416http://doi.org/10.1103/PhysRevA.93.063416 .

H. T. Hu , 等 . Wavelength and intensity effects on the dissociation of H2+ in intense laser fields . Phys. Rev. A , 2016 . 94 053415 DOI:10.1103/PhysRevA.94.053415http://doi.org/10.1103/PhysRevA.94.053415 .

Q. Y. Ji , 等 . Timing dissociative ionization of H2 using a polarization-skewed femtosecond laser pulse . Phys. Rev. Lett. , 2019 . 123 233202 DOI:10.1103/PhysRevLett.123.233202http://doi.org/10.1103/PhysRevLett.123.233202 .

S. Kangaparambil , 等 . Generalized phase sensitivity of directional bond breaking in the laser-molecule interaction . Phys. Rev. Lett. , 2020 . 125 023202 DOI:10.1103/PhysRevLett.125.023202http://doi.org/10.1103/PhysRevLett.125.023202 .

Y. H. Mi , 等 . Clocking enhanced ionization of hydrogen molecules with rotational wave packets . Phys. Rev. Lett. , 2020 . 125 173201 DOI:10.1103/PhysRevLett.125.173201http://doi.org/10.1103/PhysRevLett.125.173201 .

C. X. He , 等 . Laser-wavelength and intensity dependence of electron-nuclear energy sharing in dissociative ionization of H2 . Phys. Rev. A , 2020 . 101 053403 DOI:10.1103/PhysRevA.101.053403http://doi.org/10.1103/PhysRevA.101.053403 .

H. Liang , L. Y. Peng . Quantitative theory for electron-nuclear energy sharing in molecular ionization . Phys. Rev. A , 2020 . 101 053404 DOI:10.1103/PhysRevA.101.053404http://doi.org/10.1103/PhysRevA.101.053404 .

P. K. Cao , 等 . Resolving the time evolution of the dissociative nuclear wave packet in the repulsive state of H2+ via wave-packet interference . Phys. Rev. A , 2022 . 105 043116 DOI:10.1103/PhysRevA.105.043116http://doi.org/10.1103/PhysRevA.105.043116 .

K. Sändig , H. Figger , T. W. Hänsch . Dissociation dynamics of H2+ in intense laser fields: investigation of photofragments from single vibrational levels . Phys. Rev. Lett. , 2000 . 85 4876 -4879 . DOI:10.1103/PhysRevLett.85.4876http://doi.org/10.1103/PhysRevLett.85.4876 .

J. Wu , 等 . Electron-nuclear energy sharing in above-threshold multiphoton dissociative ionization of H2 . Phys. Rev. Lett. , 2013 . 111 023002 DOI:10.1103/PhysRevLett.111.023002http://doi.org/10.1103/PhysRevLett.111.023002 .

P. F. Lu , 等 . Electron-nuclear correlation in above-threshold double ionization of molecules . Phys. Rev. A , 2017 . 95 033404 DOI:10.1103/PhysRevA.95.033404http://doi.org/10.1103/PhysRevA.95.033404 .

Scully, M. O. & Zubairy, M. S. Quantum Optics 151–154 (Cambridge University Press, Cambridge, 1997).

S. Z. Pan , 等 . Low-energy protons in strong-field dissociation of H2+ via dipole-transitions at large bond lengths . Ultrafast Sci. , 2022 . 2022 9863548 DOI:10.34133/2022/9863548http://doi.org/10.34133/2022/9863548 .

S. I. Chu . Floquet theory and complex quasivibrational energy formalism for intense field molecular photodissociation . J. Chem. Phys. , 1981 . 75 2215 -2221 . DOI:10.1063/1.442334http://doi.org/10.1063/1.442334 .

S. I. Chu , D. A. Telnov . Beyond the Floquet theorem: generalized Floquet formalisms and quasienergy methods for atomic and molecular multiphoton processes in intense laser fields . Phys. Rep. , 2004 . 390 1 -131 . DOI:10.1016/j.physrep.2003.10.001http://doi.org/10.1016/j.physrep.2003.10.001 .

A. Giusti-Suzor , 等 . Above-threshold dissociation of H2+ in intense laser fields . Phys. Rev. Lett. , 1990 . 64 515 -518 . DOI:10.1103/PhysRevLett.64.515http://doi.org/10.1103/PhysRevLett.64.515 .

A. Zavriyev , 等 . Ionization and dissociation of H2 in intense laser fields at 1.064 μm, 532 nm, and 355 nm . Phys. Rev. A , 1990 . 42 5500 -5513 . DOI:10.1103/PhysRevA.42.5500http://doi.org/10.1103/PhysRevA.42.5500 .

G. Jolicard , O. Atabek . Above-threshold-dissociation dynamics of H2+ with short intense laser pulses . Phys. Rev. A , 1992 . 46 5845 -5855 . DOI:10.1103/PhysRevA.46.5845http://doi.org/10.1103/PhysRevA.46.5845 .

L. J. Frasinski , 等 . Counterintuitive alignment of H2+ in intense femtosecond laser fields . Phys. Rev. Lett. , 2001 . 86 2541 -2544 . DOI:10.1103/PhysRevLett.86.2541http://doi.org/10.1103/PhysRevLett.86.2541 .

A. Giusti-Suzor , F. H. Mies . Vibrational trapping and suppression of dissociation in intense laser fields . Phys. Rev. Lett. , 1992 . 68 3869 -3872 . DOI:10.1103/PhysRevLett.68.3869http://doi.org/10.1103/PhysRevLett.68.3869 .

L. J. Frasinski , 等 . Manipulation of bond hardening in H2+ by chirping of intense femtosecond laser pulses . Phys. Rev. Lett. , 1999 . 83 3625 -3628 . DOI:10.1103/PhysRevLett.83.3625http://doi.org/10.1103/PhysRevLett.83.3625 .

E. Charron , A. Giusti-Suzor , F. H. Mies . Coherent control of photodissociation in intense laser fields . J. Chem. Phys. , 1995 . 103 7359 -7373 . DOI:10.1063/1.470308http://doi.org/10.1063/1.470308 .

R. Kosloff , H. Tal-Ezer . A direct relaxation method for calculating eigenfunctions and eigenvalues of the Schrödinger equation on a grid . Chem. Phys. Lett. , 1986 . 127 223 -230 . DOI:10.1016/0009-2614(86)80262-7http://doi.org/10.1016/0009-2614(86)80262-7 .

Press, W. H. et al. Numerical Recipes: The Art of Scientific Computing. 3rd edn, 1048–1049 (Cambridge University Press, 2007).

B. Feuerstein , U. Thumm . Fragmentation of H2+ in strong 800-nm laser pulses: initial-vibrational-state dependence . Phys. Rev. A , 2003 . 67 043405 DOI:10.1103/PhysRevA.67.043405http://doi.org/10.1103/PhysRevA.67.043405 .

R. Dörner , 等 . Cold target recoil ion momentum spectroscopy: a 'momentum microscope' to view atomic collision dynamics . Phys. Rep. , 2000 . 330 95 -192 . DOI:10.1016/S0370-1573(99)00109-Xhttp://doi.org/10.1016/S0370-1573(99)00109-X .

J. Ullrich , 等 . Recoil-ion and electron momentum spectroscopy: reaction-microscopes . Rep. Prog. Phys. , 2003 . 66 1463 -1545 . DOI:10.1088/0034-4885/66/9/203http://doi.org/10.1088/0034-4885/66/9/203 .

浏览量

Downloads

CSCD

文章被引用时，请邮件提醒。

Submit

工具集

关联资源

Light | 强场驱动分子解离中的拉比振荡

暂无数据