Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Log inSign up
Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Blog
Job Board
Q3AS

© 2026 Aqora Quantum S.A.S.

TermsPrivacyLegal Notice

Acta Physica Sinica

Photoassociation reaction of H+D+ in two chirped pulses

Niu Ying-Yu, Rong Wang, Jun-Ling Xiu

Published Jan 1, 2011• 4 citations
Publisher

Abstract

The photoassociation reaction H+D+ induced by two chirped pulses is theoretically studied. The first pulse is employed to accelerate the collision pairs, and the second pulse is used to enhance the yield ratio of HD+. The optimal parameters of the second pulse and the population of product HD+ depend on the chirp rate of the first pulse. The population of the product HD+ can be controlled by the delay time between the two laser pulses.

DOI
10.7498/aps.60.123402

Related papers

Photoassociation Reactions H+D + and H + +D in Ultrashort Pulse Laser Fields

Niu Ying-Yu, Rong Wang, Libo Liu +1 more

The photoassociation reactions H+D + and H + +D induced by the one- and two-colour laser pulses are theoretically studied. The reactions occur through two channels: (i) H(1S)+D + → HD + , and (ii) H + +D(1S) → HD + . The reaction probability through channel (ii) is higher than through channel (i). The populations of the products H + +D and HD + and the ratio of H + +D to HD + can be controlled by laser pulses. The two-colour laser pulses can more efficiently lower the dissociation probability and therefore enhance the yield ratio of the product HD + .

Chinese Physics Letters•Dec 1, 2007•8 citations

Control of photoassociation reaction F+H→HF with ultrashort laser pulse

Libo Liu, Niu Ying-Yu, Kai‐Jun Yuan +1 more

The laser-induced vibrational state-selectivity of product HF in photoassociation reaction H+F→HF is theoretically investigated by using the time-dependent quantum wave packet method. The population transfer process from the continuum state down to the bound vibrational states can be controlled by the driving laser. The effects of laser pulse parameters and the initial momentum of the two collision atoms on the vibrational population of the product HF are discussed in detail. Photodissociation accompanied with the photoassociation process is also described.

Chinese Physics•Oct 1, 2007•16 citations

Coherent control of cold-molecule formation through photoassociation using a chirped-pulsed-laser field

Jiří Vala, Olivier Dulieu, Françoise Masnou-Seeuws +2 more

Enhancement of the production of cold molecules via photoassociation is considered for the ${\mathrm{Cs}}_{2}$ system. The employment of chirped picosecond pulses is proposed and studied theoretically. The analysis is based on the ability to achieve impulsive excitation which is given by the ultracold initial conditions where the nuclei are effectively stationary during the interaction with a field. The appropriate theoretical framework is the coordinate-dependent two-level system. Matching the pulse parameters to the potentials and initial conditions results in full Rabi cycling between the electronic potentials. By chirping the laser pulse, adiabatic transfer leading to the population inversion from the ground to the excited state is possible in a broad and tunable range of internuclear distance. Numerical simulations based on solving the time-dependent Schr\"odinger equation (TDSE) were performed. The simulation of the photoassociation of ${\mathrm{Cs}}_{2}$ from the ground ${}^{3}{\ensuremath{\Sigma}}_{u}^{+}$ to the excited ${0}_{g}^{\ensuremath{-}}$ state under ultracold conditions verifies the qualitative picture. The ability to control the population transfer is employed to optimize molecular formation. Transfer of population to the excited ${0}_{g}^{\ensuremath{-}}$ surface leaves a void in the nuclear density of the ground ${}^{3}{\ensuremath{\Sigma}}_{u}^{+}$ surface. This void is either filled by thermal motion or by quantum ``pressure'' and it is the rate-determining step in the photoassociation. The spontaneous-emission process leading to cold-molecules is simulated by including an optical potential in the TDSE. Consequently, the rate of cold molecule formation in a pulsed mode is found to be larger than that obtained in a continuous-wave mode.

Physical Review A•Dec 12, 2000•107 citations

Photoassociation of cold atoms with chirped laser pulses: Time-dependent calculations and analysis of the adiabatic transfer within a two-state model

Eliane Luc-Koenig, Ronnie Kosloff, Françoise Masnou-Seeuws +1 more

This theoretical paper presents numerical calculations for the photoassociation of ultracold cesium atoms with a chirped laser pulse and a detailed analysis of the results. In contrast with earlier work, the initial state is represented by a stationary continuum wave function. In the chosen example, it is shown that an important population transfer is achieved to $\ensuremath{\approx}15$ vibrational levels in the vicinity of the $v=98$ bound level in the external well of the ${0}_{g}^{\ensuremath{-}}(6s+6{p}_{3∕2})$ potential. Such levels lie in the energy range swept by the instantaneous frequency of the pulse, thus defining a ``photoassociation window.'' Levels outside this window may be significantly excited during the pulse, but no population remains there after the pulse. Finally, the population transfer to the last vibrational levels of the ground $a\phantom{\rule{0.2em}{0ex}}^{3}\ensuremath{\sum}_{u}^{+}(6\mathrm{s}+6\mathrm{s})$ state is significant, making stable molecules. The results are interpreted in the framework of a two-state model as an adiabatic inversion mechanism, efficient only within the photoassociation window. The large value found for the photoassociation rate suggests promising applications. The present chirp has been designed in view of creating in the excited state a vibrational wave packet that is focusing at the barrier of the double-well potential.

arXiv:physics/0404028•Physical Review A•Sep 27, 2004•107 citations

Control of Chemical Reactions by Using Chirped Laser Pulses

Junici Shimamura, Kenji Mishima, Koichi Yamashita

Quantum wavepacket calculations have been performed to study ways of using chirped laser pulses to control (a) complete population transfer, (b) coherent Raman processes, and (c) vibrational cooling via photoassociation. It has been found that positively and negatively chirped pulses significantly influence the behavior of wavepackets for these elementary processes. Although some of the numerical results can be interpreted from the standpoint of intra-pulse pump-dump processes, we have discovered some novel characteristics of chirped pulses.

ACS symposium series•Jun 21, 2002•0 citations

Coherent control of bond making: the performance of rationally phase-shaped femtosecond laser pulses*

Liat Levin, Wojciech Skomorowski, Ronnie Kosloff +2 more

Abstract The first step in the coherent control of a photoinduced binary reaction is bond making or photoassociation. We have recently demonstrated coherent control of bond making in multi-photon femtosecond photoassociation of hot magnesium atoms, using linearly chirped pulses (Levin et al 2015 Phys. Rev. Lett. 114 233003 ). The detected yield of photoassociated magnesium dimers was enhanced by positively chirped pulses which is explained theoretically by a combination of purification and chirp-dependent Raman transitions. The yield could be further enhanced by pulse optimization resulting in pulses with an effective linear chirp and a sub-pulse structure, where the latter allows for exploiting vibrational coherences. Here, we systematically explore the efficiency of phase-shaped pulses for the coherent control of bond making, employing a parametrization of the spectral phases in the form of cosine functions. We find up to an order of magnitude enhancement of the yield compared to the unshaped transform-limited pulse. The highly performing pulses all display an overall temporally increasing instantaneous frequency and are composed of several overlapping sub-pulses. The time delay between the first two sub-pulses fits very well the vibrational frequency of the generated intermediate wavepacket. These findings are in agreement with chirp-dependent Raman transitions and exploitation of vibrational dynamics as underlying control mechanisms.

arXiv:1505.04976•Journal of Physics B Atomic Molecular and Optical Physics•Jul 29, 2015•11 citations
The photoassociation reaction H+D+ induced by two chirped pulses is theoretically studied. The first pulse is employed to accelerate the collision pairs, and the second pulse is used to enhance the yield ratio of HD+. The optimal parameters of the second pulse and the population of product HD+ depend on the chirp rate of the first pulse. The population of the product HD+ can be controlled by the delay time between the two laser pulses.
The photoassociation reactions H+D + and H + +D induced by the one- and two-colour laser pulses are theoretically studied. The reactions occur through two channels: (i) H(1S)+D + → HD + , and (ii) H + +D(1S) → HD + . The reaction probability through channel (ii) is higher than through channel (i). The populations of the products H + +D and HD + and the ratio of H + +D to HD + can be controlled by laser pulses. The two-colour laser pulses can more efficiently lower the dissociation probability and therefore enhance the yield ratio of the product HD + .
The laser-induced vibrational state-selectivity of product HF in photoassociation reaction H+F→HF is theoretically investigated by using the time-dependent quantum wave packet method. The population transfer process from the continuum state down to the bound vibrational states can be controlled by the driving laser. The effects of laser pulse parameters and the initial momentum of the two collision atoms on the vibrational population of the product HF are discussed in detail. Photodissociation accompanied with the photoassociation process is also described.
Enhancement of the production of cold molecules via photoassociation is considered for the Cs2{\mathrm{Cs}}_{2}Cs2​ system. The employment of chirped picosecond pulses is proposed and studied theoretically. The analysis is based on the ability to achieve impulsive excitation which is given by the ultracold initial conditions where the nuclei are effectively stationary during the interaction with a field. The appropriate theoretical framework is the coordinate-dependent two-level system. Matching the pulse parameters to the potentials and initial conditions results in full Rabi cycling between the electronic potentials. By chirping the laser pulse, adiabatic transfer leading to the population inversion from the ground to the excited state is possible in a broad and tunable range of internuclear distance. Numerical simulations based on solving the time-dependent Schr\"odinger equation (TDSE) were performed. The simulation of the photoassociation of Cs2{\mathrm{Cs}}_{2}Cs2​ from the ground ${}^{3}{\ensuremath{\Sigma}}_{u}^{+}$ to the excited ${0}_{g}^{\ensuremath{-}}$ state under ultracold conditions verifies the qualitative picture. The ability to control the population transfer is employed to optimize molecular formation. Transfer of population to the excited ${0}_{g}^{\ensuremath{-}}$ surface leaves a void in the nuclear density of the ground ${}^{3}{\ensuremath{\Sigma}}_{u}^{+}$ surface. This void is either filled by thermal motion or by quantum ``pressure'' and it is the rate-determining step in the photoassociation. The spontaneous-emission process leading to cold-molecules is simulated by including an optical potential in the TDSE. Consequently, the rate of cold molecule formation in a pulsed mode is found to be larger than that obtained in a continuous-wave mode.
This theoretical paper presents numerical calculations for the photoassociation of ultracold cesium atoms with a chirped laser pulse and a detailed analysis of the results. In contrast with earlier work, the initial state is represented by a stationary continuum wave function. In the chosen example, it is shown that an important population transfer is achieved to $\ensuremath{\approx}15$ vibrational levels in the vicinity of the v=98v=98v=98 bound level in the external well of the ${0}_{g}^{\ensuremath{-}}(6s+6{p}_{3∕2})$ potential. Such levels lie in the energy range swept by the instantaneous frequency of the pulse, thus defining a ``photoassociation window.'' Levels outside this window may be significantly excited during the pulse, but no population remains there after the pulse. Finally, the population transfer to the last vibrational levels of the ground $a\phantom{\rule{0.2em}{0ex}}^{3}\ensuremath{\sum}_{u}^{+}(6\mathrm{s}+6\mathrm{s})$ state is significant, making stable molecules. The results are interpreted in the framework of a two-state model as an adiabatic inversion mechanism, efficient only within the photoassociation window. The large value found for the photoassociation rate suggests promising applications. The present chirp has been designed in view of creating in the excited state a vibrational wave packet that is focusing at the barrier of the double-well potential.
Quantum wavepacket calculations have been performed to study ways of using chirped laser pulses to control (a) complete population transfer, (b) coherent Raman processes, and (c) vibrational cooling via photoassociation. It has been found that positively and negatively chirped pulses significantly influence the behavior of wavepackets for these elementary processes. Although some of the numerical results can be interpreted from the standpoint of intra-pulse pump-dump processes, we have discovered some novel characteristics of chirped pulses.
Abstract The first step in the coherent control of a photoinduced binary reaction is bond making or photoassociation. We have recently demonstrated coherent control of bond making in multi-photon femtosecond photoassociation of hot magnesium atoms, using linearly chirped pulses (Levin et al 2015 Phys. Rev. Lett. 114 233003 ). The detected yield of photoassociated magnesium dimers was enhanced by positively chirped pulses which is explained theoretically by a combination of purification and chirp-dependent Raman transitions. The yield could be further enhanced by pulse optimization resulting in pulses with an effective linear chirp and a sub-pulse structure, where the latter allows for exploiting vibrational coherences. Here, we systematically explore the efficiency of phase-shaped pulses for the coherent control of bond making, employing a parametrization of the spectral phases in the form of cosine functions. We find up to an order of magnitude enhancement of the yield compared to the unshaped transform-limited pulse. The highly performing pulses all display an overall temporally increasing instantaneous frequency and are composed of several overlapping sub-pulses. The time delay between the first two sub-pulses fits very well the vibrational frequency of the generated intermediate wavepacket. These findings are in agreement with chirp-dependent Raman transitions and exploitation of vibrational dynamics as underlying control mechanisms.