A femtosecond laser pulse can be tailored to control the two-photon transitions using the ultra-fast pulse-shaping technique. This paper theoretically and experimentally demonstrates that two-photon transitions in mol...A femtosecond laser pulse can be tailored to control the two-photon transitions using the ultra-fast pulse-shaping technique. This paper theoretically and experimentally demonstrates that two-photon transitions in molecular system with broad absorption line can be effectively controlled by square phase-modulation in frequency domain, and the influence of all parameters characterizing the square phase-modulation on two-photon transitions is systemically investigated and discussed. The obtained results have potential application in nonlinear spectroscopy and molecular physics.展开更多
In this paper, we study theoretically and experimentally the coherent control of non-resonant two-photon transition in a molecular system （Perylene dissolved in chloroform solution） by shaping the femtosecond pulses...In this paper, we study theoretically and experimentally the coherent control of non-resonant two-photon transition in a molecular system （Perylene dissolved in chloroform solution） by shaping the femtosecond pulses with simple phase patterns （cosinusoidal and π phase step-function shape）. The control efficiency of the two-photon transition probability is correlated with both the laser field and the molecular absorption bandwidth. Our results demonstrate that, the two-photon transition probability in a molecular system can be reduced but not completely eliminated by manipulating the laser field, and the control efficiency is minimal when the molecular absorption bandwidth is larger than twice the laser spectral bandwidth.展开更多
We experimentally observe the high resolution direct frequency comb spectroscopy using counter-propagating broadband femtosecond pulses on two-photon transitions in room-temperature ^87 Rb atoms. The Doppler broad- en...We experimentally observe the high resolution direct frequency comb spectroscopy using counter-propagating broadband femtosecond pulses on two-photon transitions in room-temperature ^87 Rb atoms. The Doppler broad- ened background is effectively eliminated with the pulse shaping method and the spectrum modulation technique. The combination of the pulse shaping method and the spectra modulation technique provides a potential approachto reduce background of at least 99%.展开更多
The strong-field coherent control of the nonresonant ionization of nitrous oxide using shaped pulses is investigated.We study the dependence of periodic coherent oscillation of the total ionization yield on the variat...The strong-field coherent control of the nonresonant ionization of nitrous oxide using shaped pulses is investigated.We study the dependence of periodic coherent oscillation of the total ionization yield on the variation of laser phase parameters. The physical mechanism of the strong-field coherent control is investigated experimentally and theoretically by the nonresonant spectral phase interferences in the frequency domain. We show that the intense shaped pulses with broadband and off-resonance can be used as a robust strong-field coherent control method.展开更多
Coherent control of fragmentation of CH_3I using shaped femtosecond pulse train is investigated.The dissociation processes can be modulated by changing the separation of the shaped pulse train, and the yield of I^+und...Coherent control of fragmentation of CH_3I using shaped femtosecond pulse train is investigated.The dissociation processes can be modulated by changing the separation of the shaped pulse train, and the yield of I^+under the irradiation of the optimal pulse is significantly increased compared with that using the transform-limited pulse.We discuss the control mechanism of dissociation processes with coherent interference in time domain.A three-pulse control model is proposed to explain the counterintuitive experimental results.展开更多
A train of three equally spaced femtosecond laser pulses is employed to control the photoionization/photodissociation processes of cyclopentanone. With the increase of pulse separation, a strong modulation of product ...A train of three equally spaced femtosecond laser pulses is employed to control the photoionization/photodissociation processes of cyclopentanone. With the increase of pulse separation, a strong modulation of product ion yield is observed. More than ten-fold changes of ion yield ratio between different products can be realized. The experimental observations further explain the compositions and formation pathways of peaks in the mass spectra. The controlling mechanisms are also discussed.展开更多
Improving the up-conversion luminescence efficiency crucial in several related application areas. In this work, of rare-earth ions via the multi-photon absorption process is we theoretically propose a feasible scheme ...Improving the up-conversion luminescence efficiency crucial in several related application areas. In this work, of rare-earth ions via the multi-photon absorption process is we theoretically propose a feasible scheme to enhance the resonance-mediated two-photon absorption in Er3＋ ions by shaping the femtosecond laser field with a rectangle phase modulation. Our theoretical results show that the resonance-mediated two-photon absorption can be decomposed into the on-resonant and near-resonant parts, and the on-resonant part mainly comes from the contribution of laser central frequency components, while the near-resonant part mainly results from the excitation of low and high laser frequency components. So, the rectangle phase modulation can induce a constructive interference between the two parts by properly designing the modulation depth and width, and finally realizes the resonance-mediated two-photon absorption enhancement. More- over, our results also show that the enhancement efficiency of resonance-mediated two-photon absorption depends on the laser pulse width （or laser spectral bandwidth）, final state transition frequency, and intermediate and final state absorption bandwidths. The enhancement efficiency modulation can be attributed to the relative weight manipulation of on-resonant and near-resonant two-photon absorption in the whole excitation process. This study presents a clear physical insight for the quantum control of resonance-mediated two-photon absorption in the rare-earth ions, and there will be an important significance for improving the up-conversion luminescence efficiency of rare-earth ions.展开更多
Enhancing the upconversion luminescence of rare earth ions is crucial for their applications in the laser sources,fiber optic communications,color displays,biolabeling,and biomedical sensors.In this paper,we theoretic...Enhancing the upconversion luminescence of rare earth ions is crucial for their applications in the laser sources,fiber optic communications,color displays,biolabeling,and biomedical sensors.In this paper,we theoretically study the resonance-mediated(1+2)-three-photon absorption in Pr^(3+) ions by a rectangle phase modulation.The results show that the resonance-mediated(1+2)-three-photon absorption can be effectively enhanced by properly designing the depth and width of the rectangle phase modulation,which can be attributed to the constructive interference between on-resonant and near-resonant three-photon excitation pathways.Further,the enhancement efficiency of resonance-mediated(1+2)-threephoton absorption can be affected by the pulse width(or spectral bandwidth)of femtosecond laser field,final state transition frequency,and absorption bandwidths.This research can provide a clear physical picture for understanding and controlling the multi-photon absorption in rare-earth ions,and also can provide theoretical guidance for improving the up-conversion luminescence.展开更多
基金supported by the National Natural Science Foundation of China (Grant No 10574046)National Key Project for Basic Research of China (Grant Nos 2006CB806006 and 2006CB921105)+2 种基金Program for Changjiang Scholars and Innovative Research Team in University (PCSIRT), Program for New Century Excellent Talents in University (NCET-04-0420)the Doctoral Program of High Education (Grant No 20050269011)Phosphor Program sponsored by Shanghai Science and Technology Committee (Grant No 06QH14003)
文摘A femtosecond laser pulse can be tailored to control the two-photon transitions using the ultra-fast pulse-shaping technique. This paper theoretically and experimentally demonstrates that two-photon transitions in molecular system with broad absorption line can be effectively controlled by square phase-modulation in frequency domain, and the influence of all parameters characterizing the square phase-modulation on two-photon transitions is systemically investigated and discussed. The obtained results have potential application in nonlinear spectroscopy and molecular physics.
基金Project supported by Shanghai Leading Academic Discipline Project (Grant No. B408)National Key Program for Basic Research of China (Grant Nos. 2006CB806006 and 2006CB921105)+1 种基金Ministry of Education of China (Grant No. 30800)Shanghai Municipal Science and Technology Commission (Grant Nos. 07DZ22025,09142200501 and 09ZR1409300)
文摘In this paper, we study theoretically and experimentally the coherent control of non-resonant two-photon transition in a molecular system （Perylene dissolved in chloroform solution） by shaping the femtosecond pulses with simple phase patterns （cosinusoidal and π phase step-function shape）. The control efficiency of the two-photon transition probability is correlated with both the laser field and the molecular absorption bandwidth. Our results demonstrate that, the two-photon transition probability in a molecular system can be reduced but not completely eliminated by manipulating the laser field, and the control efficiency is minimal when the molecular absorption bandwidth is larger than twice the laser spectral bandwidth.
基金Supported by the National Basic Research Program of China under Grant No 2012CB921603the Program for Changjiang Scholars and Innovative Research Team in University of Ministry of Education of China under Grant No IRT13076the National Natural Science Foundation of China under Grant Nos 61378049,10934004,11404198,61575116 and 61505100
文摘We experimentally observe the high resolution direct frequency comb spectroscopy using counter-propagating broadband femtosecond pulses on two-photon transitions in room-temperature ^87 Rb atoms. The Doppler broad- ened background is effectively eliminated with the pulse shaping method and the spectrum modulation technique. The combination of the pulse shaping method and the spectra modulation technique provides a potential approachto reduce background of at least 99%.
基金supported by the National Natural Science Foundation of China(Grant No.11374124)
文摘The strong-field coherent control of the nonresonant ionization of nitrous oxide using shaped pulses is investigated.We study the dependence of periodic coherent oscillation of the total ionization yield on the variation of laser phase parameters. The physical mechanism of the strong-field coherent control is investigated experimentally and theoretically by the nonresonant spectral phase interferences in the frequency domain. We show that the intense shaped pulses with broadband and off-resonance can be used as a robust strong-field coherent control method.
基金Project supported by the National Natural Science Foundation of China(Grant No.11374124)
文摘Coherent control of fragmentation of CH_3I using shaped femtosecond pulse train is investigated.The dissociation processes can be modulated by changing the separation of the shaped pulse train, and the yield of I^+under the irradiation of the optimal pulse is significantly increased compared with that using the transform-limited pulse.We discuss the control mechanism of dissociation processes with coherent interference in time domain.A three-pulse control model is proposed to explain the counterintuitive experimental results.
基金Project supported by the National Basic Research Program of China (973 Program) (Grant No.2013CB922200)the National Natural Science Foundation of China,(Grant Nos.10774056 and 10974070)+1 种基金the Fundamental Research Funds for the Central Universities,China (Grant No.200903371)the Specialized Research Fund for the Doctoral Program of Higher Education,China (Grant No.20100061110045)
文摘A train of three equally spaced femtosecond laser pulses is employed to control the photoionization/photodissociation processes of cyclopentanone. With the increase of pulse separation, a strong modulation of product ion yield is observed. More than ten-fold changes of ion yield ratio between different products can be realized. The experimental observations further explain the compositions and formation pathways of peaks in the mass spectra. The controlling mechanisms are also discussed.
基金Project supported by the National Natural Science Foundation of China(Grant No.11474096)the Science and Technology Commission of Shanghai Municipality,China(Grant Nos.14JC1401500,17ZR146900,and 16520721200)the Higher Education Key Program of He'nan Province of China(Grant No.17A140025)
文摘Improving the up-conversion luminescence efficiency crucial in several related application areas. In this work, of rare-earth ions via the multi-photon absorption process is we theoretically propose a feasible scheme to enhance the resonance-mediated two-photon absorption in Er3＋ ions by shaping the femtosecond laser field with a rectangle phase modulation. Our theoretical results show that the resonance-mediated two-photon absorption can be decomposed into the on-resonant and near-resonant parts, and the on-resonant part mainly comes from the contribution of laser central frequency components, while the near-resonant part mainly results from the excitation of low and high laser frequency components. So, the rectangle phase modulation can induce a constructive interference between the two parts by properly designing the modulation depth and width, and finally realizes the resonance-mediated two-photon absorption enhancement. More- over, our results also show that the enhancement efficiency of resonance-mediated two-photon absorption depends on the laser pulse width （or laser spectral bandwidth）, final state transition frequency, and intermediate and final state absorption bandwidths. The enhancement efficiency modulation can be attributed to the relative weight manipulation of on-resonant and near-resonant two-photon absorption in the whole excitation process. This study presents a clear physical insight for the quantum control of resonance-mediated two-photon absorption in the rare-earth ions, and there will be an important significance for improving the up-conversion luminescence efficiency of rare-earth ions.
基金supported by the National Natural Science Foundation of China(Grant Nos.12004238 and 11764036)the Natural Science Foundation of Henan Province,China(Grant No.222102230068)the Open Subject of the Key Laboratory of Weak Light Nonlinear Photonics of Nankai University(Grant No.OS 21-3)。
文摘Enhancing the upconversion luminescence of rare earth ions is crucial for their applications in the laser sources,fiber optic communications,color displays,biolabeling,and biomedical sensors.In this paper,we theoretically study the resonance-mediated(1+2)-three-photon absorption in Pr^(3+) ions by a rectangle phase modulation.The results show that the resonance-mediated(1+2)-three-photon absorption can be effectively enhanced by properly designing the depth and width of the rectangle phase modulation,which can be attributed to the constructive interference between on-resonant and near-resonant three-photon excitation pathways.Further,the enhancement efficiency of resonance-mediated(1+2)-threephoton absorption can be affected by the pulse width(or spectral bandwidth)of femtosecond laser field,final state transition frequency,and absorption bandwidths.This research can provide a clear physical picture for understanding and controlling the multi-photon absorption in rare-earth ions,and also can provide theoretical guidance for improving the up-conversion luminescence.
基金Supported by National Natural Science Foundation of China(11474096,11604199,11747101)Natural Science Foundation of Henan Province(182102210117,17A140025,16A140030)Science and Technology Commission of Shanghai Municipality(14JC1401500)~~
