Molecular orbital imaging via above-threshold ionization with circularly polarized pulses

Zhu, Xinxin; Zhang, Qingbin; Hong, Weiyi; Lu, Peixiang; Xu, Zhizhan

doi:10.1364/oe.19.013722

Cited by 28 publications

(14 citation statements)

References 30 publications

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“…For instance, this HHG process offers an ideal framework for the study of strong-field dynamics [37]. Moreover, as the CPLP has already shown its great power in the application of (one-shot) imaging or structure detection of molecules [39][40][41][42], the HHG by CPLP can be potentially utilized for the imaging and detection of molecules with an all-optical method.…”

Section: Discussionmentioning

confidence: 99%

“…It is found that the higher efficiency is mainly contributed in the recombination step and is at least partly due to the higher recollision probability for molecules. Since this HHG process involves the unique recollision mechanism under a circularly polarized laser field, it will stimulate new potential applications, such as offering an ideal framework for study of strong-field dynamics [37] and (one-shot) imaging or structure detection of molecules with all optical methods [39][40][41][42].…”

Section: Introductionmentioning

confidence: 99%

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Molecular high-order-harmonic generation due to the recollision mechanism by a circularly polarized laser pulse

et al. 2015

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High-order-harmonic generation (HHG) from small linear molecules driven by a circularly polarized laser pulse (CPLP) is investigated. It is found that the obtained high-order harmonics are more pronounced than those from reference atoms with equal ionization potential driven by the same CPLP. By analyzing the dependence of the cutoff position on laser parameters and calculating the recollision trajectories, it is shown that this molecular HHG originates from the recollision mechanism, instead of the bound-bound transition mechanism found to be responsible for molecular HHG by CPLP in earlier works. A semiclassical model is used to analyze the HHG process and discuss the origin of the higher efficiency of molecular HHG. It is found that the higher HHG efficiency for molecules is mainly contributed in the recombination step and at least partly due to the higher recollision probability of continuum electrons.

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Section: Discussionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Molecular high-order-harmonic generation due to the recollision mechanism by a circularly polarized laser pulse

et al. 2015

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“…Alternatively, PMDs can be measured in a reaction microscope [22], where information on the molecular orientation is obtained by electron-ion coincidence. For molecular imaging, circularly polarized light effectively delivers a 360°scan of the aligned molecule [23][24][25], which is an advantage over linear polarization. In the classical trajectory model without Coulomb effects, electrons measured at an emission angle ϕ originate from ionization at the angle ϕ AE 90°with the sign depending on the rotation direction of the field.…”

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confidence: 99%

“…We use a 800 nm wavelength and a constant amplitude E 0 corresponding to an intensity of I ¼ 2.5 × 10 14 W=cm 2 , unless specified otherwise. Choosing a continuous wave (cw) field has the following reasons: (i) multicycle pulses avoid anisotropies introduced by the pulse envelope and thus bring out the angle-dependent ionization probability of the molecular orbital [24] and (ii) the cw field reduces the numerical workload.…”

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Signatures of Molecular Orbital Structure in Lateral Electron Momentum Distributions from Strong-Field Ionization

2015

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Strong-field ionization of aligned diatomic and polyatomic molecules such as O 2 , N 2 , C 2 H 4 , and others in circularly polarized laser fields is investigated theoretically. By calculating the emission-angle-resolved lateral width of the momentum distribution perpendicular to the polarization plane, we show that nodal planes in molecular orbitals are directly imprinted on the angular dependence of the width. We demonstrate that orbital symmetries can be distinguished with the information obtained by observing the lateral width in addition to the angular distributions. DOI: 10.1103/PhysRevLett.114.103004 PACS numbers: 33.80.Rv, 33.20.Xx Progress in strong-field science has led to the possibility to image dynamics in atoms and molecules on the attosecond time scale and angstrom spatial scale [1][2][3]. Laser-based methods to image molecular structure include diffraction of recolliding electrons [4][5][6], Coulomb explosion imaging [7,8], and orbital tomography [9][10][11][12][13][14]. Information about the orbital structure of aligned molecules is also contained in the dependence of the ionization rate on the angle between the laser polarization direction and the molecular axis [15,16] with particular care needed for polar molecules [17]. Rich information is obtained by measuring three-dimensional photoelectron momentum distributions (PMDs) of aligned molecules. This is possible by combining laser-induced alignment of molecules [18,19] and velocity-map imaging [20,21]. Alternatively, PMDs can be measured in a reaction microscope [22], where information on the molecular orientation is obtained by electron-ion coincidence. For molecular imaging, circularly polarized light effectively delivers a 360°scan of the aligned molecule [23][24][25], which is an advantage over linear polarization. In the classical trajectory model without Coulomb effects, electrons measured at an emission angle ϕ originate from ionization at the angle ϕ AE 90°with the sign depending on the rotation direction of the field. Another advantage of circular polarization is the absence of electron recollisions that could obscure the measured distribution. Nodal structures have been measured successfully for various molecules using many-cycle circularly polarized pulses [26][27][28][29]. Theoretical prediction of the PMDs is complicated by the nonperturbative nature of the ionization process in the commonly used near-infrared fields. Only for very small molecules such as H 2 þ [30] or in proof-of-principle calculations with model orbitals [31], the solution of the timedependent Schrödinger equation (TDSE) is an option. In contrast, the strong-field approximation (SFA) can be used to calculate PMDs of arbitrary molecules and often yields accurate results [32][33][34]. In polar molecules, an extended SFA including the Stark shift is beneficial [35][36][37].To the authors' knowledge, none of the published experimental work on molecular imaging has made use of the lateral photoelectron momentum distribution (LPMD), i.e., the distribution of the m...

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“…There are also other forms of polarizations, the circular and elliptical polarizations, which still involve abundant topics to be studied. Investigations on the PADs for both polar and non-polar molecules ionized by circularly polarized laser pulses have been performed lately [27,28,29], and very recently Abu-samha et al [30] has studied the photoelectron momentum distribution of atomic oribtals by elliptically polarized laser pulses. Nevertheless, investigations on the PADs in response to elliptically polarized exciting lasers especially from polar molecules are still in request.…”

Section: Introductionmentioning

confidence: 99%

Laser-polarization-dependent photoelectron angular distributions from polar molecules

et al. 2011

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Photoelectron angular distributions (PADs) of oriented polar molecules in response to different polarized lasers are systematically investigated. It is found that the PADs of polar CO molecules show three distinct styles excited by linearly, elliptically and circularly polarized lasers respectively. In the case of elliptical polarization, a deep suppression is observed along the major axis and the distribution concentrates approximately along the minor axis. Additionally, it is also found that the concentrated distributions rotate clockwise as the ellipticity increases. Our investigation presents a method to manipulate the motion and angular distribution of photoelectrons by varying the polarization of the exciting pulses, and also implies the possibility to control the processes in laser-molecule interactions in future work. References and links 1. P. Agostini, F. Fabre, G. Mainfray, and G. Petite, "Free-free transitions following six-photon ionization of Xenon atoms," Phys. Rev. Lett. 42, 1127Lett. 42, -1130Lett. 42, (1979. 2. C. I. Blaga, F. Catoire, P. Colosimo, G. G. Paulus, H. G. Muller, P. Agostini, and L. F. DiMauro, "Strong-field photoionization revisited," Nat. Phys. 5, 335-338 (2009

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Molecular orbital imaging via above-threshold ionization with circularly polarized pulses

Cited by 28 publications

References 30 publications

Molecular high-order-harmonic generation due to the recollision mechanism by a circularly polarized laser pulse

Molecular high-order-harmonic generation due to the recollision mechanism by a circularly polarized laser pulse

Signatures of Molecular Orbital Structure in Lateral Electron Momentum Distributions from Strong-Field Ionization

Laser-polarization-dependent photoelectron angular distributions from polar molecules

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