Second-harmonic generation(SHG)has found extensive applications from hand-held laser pointers to spectroscopic and microscopic techniques.Recently,some cleavable van der Waals(vdW)crystals have shown SHG arising from ...Second-harmonic generation(SHG)has found extensive applications from hand-held laser pointers to spectroscopic and microscopic techniques.Recently,some cleavable van der Waals(vdW)crystals have shown SHG arising from a single atomic layer,where the SH light elucidated important information such as the grain boundaries and electronic structure in these ultra-thin materials.However,despite the inversion asymmetry of the single layer,the typical crystal stacking restores inversion symmetry for even numbers of layers leading to an oscillatory SH response,drastically reducing the applicability of vdW crystals such as molybdenum disulfide(MoS_(2)).Here,we probe the SHG generated from the noncentrosymmetric 3R crystal phase of MoS_(2).We experimentally observed quadratic dependence of second-harmonic intensity on layer number as a result of atomically phase-matched nonlinear dipoles in layers of the 3R crystal that constructively interfere.By studying the layer evolution of the A and B excitonic transitions in 3R-MoS_(2) using SHG spectroscopy,we also found distinct electronic structure differences arising from the crystal structure and the dramatic effect of symmetry and layer stacking on the nonlinear properties of these atomic crystals.The constructive nature of the SHG in this 2D crystal provides a platform to reliably develop atomically flat and controllably thin nonlinear media.展开更多
Entangled photon pairs are crucial resources for quantum information processing protocols.Via the process of spontaneous parametric downconversion(SPDC),we can generate these photon pairs using bulk nonlinear crystals...Entangled photon pairs are crucial resources for quantum information processing protocols.Via the process of spontaneous parametric downconversion(SPDC),we can generate these photon pairs using bulk nonlinear crystals.Traditionally,the crystal is designed to satisfy a specific type of phase-matching condition.Here,we report controllable transitions among different types of phase matching in a single periodically poled potassium titanyl phosphate crystal.By carefully selecting pump conditions,we can satisfy different phase-matching conditions.This allows us to observe first-order Type-II,fifth-order Type-I,third-order Type-0,and fifth-order Type-II SPDCs.The temperature-dependent spectra of our source were also analyzed in detail.Finally,we discussed the possibility of observing more than nine SPDCs in this crystal.Our work not only deepens the understanding of the physics behind phase-matching conditions,but also offers the potential for a highly versatile entangled biphoton source for quantum information research.展开更多
As a promising candidate,the fluorooxoborate has enkindled new explorations of nonlinear optical materials to meet the deep-ultraviolet criteria.However,big challenges and open questions still remain facing this excit...As a promising candidate,the fluorooxoborate has enkindled new explorations of nonlinear optical materials to meet the deep-ultraviolet criteria.However,big challenges and open questions still remain facing this exciting new field,especially the birefringence and dispersion of refractive index which are fundamental parameters for determining the phasematching second harmonic generation wavelength.Here we designed possible anionic groups in fluorooxoborates,and analyzed the optical anisotropy to check its influence on birefringence,which was proved further by the response electronic distribution anisotropy approximation.The functional modules modulating birefringence in fluorooxoborates were explored systematically.We developed an approach for evaluating the behavior of the refractive index dispersions and found that the fluorooxoborates had small refractive index dispersions owing to the introduction of fluorooxoborate modules.Our results demonstrate that fluorooxoborates can be utilized to realize short phase-matching wavelength markedly and offer a path toward novel performance-driven materials design.展开更多
We investigate off-axis phase-matched terahertz(THz)radiation in laser plasma pumped by few-cycle laser pulses.We find that the THz amplitude and angular distributions in the far field are sensitively dependent on the...We investigate off-axis phase-matched terahertz(THz)radiation in laser plasma pumped by few-cycle laser pulses.We find that the THz amplitude and angular distributions in the far field are sensitively dependent on the pump pulse’s focal carrier-envelope phase(CEP).Ring-like profiles of THz radiation are obtained at CEP values of 0.5πand 1.5π,due to the inversely symmetric local THz waveforms emitted before and after laser focus.Off-axis phase-matched THz radiation offers a tool to accurately measure the CEP of few-cycle pulses at the center of a medium.展开更多
The extreme ultraviolet(XUV)light beam carrying orbital angular momentum(OAM)can be produced via high-order harmonic generation(HHG)due to the interaction of an intense vortex infrared laser and a gas medium.Here we s...The extreme ultraviolet(XUV)light beam carrying orbital angular momentum(OAM)can be produced via high-order harmonic generation(HHG)due to the interaction of an intense vortex infrared laser and a gas medium.Here we show that the OAM spectrum of vortex HHG can be readily tailored by varying the radial node(from 0 to 2)in the driving laser consisting of two mixed Laguerre-Gaussian(LG)beams.We find that due to the change in spatial profile of HHG,the distribution range of the OAM spectrum can be broadened and its shape can be modified by increasing the radial node.We also show that the OAM mode range becomes much wider and its distribution shape becomes more symmetric when the harmonic order is increased from the plateau to the cutoff when the driving laser has the nonzero radial nodes.Through the map of coherence length and the evolution of harmonic field in the medium,we reveal that the favorable off-axis phase-matching conditions are greatly modified due to the change of intensity and phase distributions of driving laser with the radial node.We anticipate this work to stimulate some interests in generating the XUV vortex beam with tunable OAM spectrum through the gaseous HHG process achieved by manipulating the mode properties of the driving laser beam.展开更多
Nonlinear optical(NLO)materials play an increasingly important role in laser technology.Birefringence is one of the most important parameters for NLO materials to realize angle phase-matching conditions.In comparison ...Nonlinear optical(NLO)materials play an increasingly important role in laser technology.Birefringence is one of the most important parameters for NLO materials to realize angle phase-matching conditions.In comparison with other desirable optical properties,the availability of birefringence and refractive index dispersion is especially problematic owing to the strict requirements for single crystals.In this review,we described how to obtain the refractive index and birefringence of NLO materials from crystals sub-millimeters to centimeters in size.Espe-cially,recently developed methods including the minimum deflection angle method,auto-collimation method,prism coupling method,oil immersion technique,interference color method,and theoretical calculation(DFT)for rapid assessment of birefringence are summarized,the contents of which are mainly focused on the principles and typical applications,together with the advantages and drawbacks.In addition,representative examples of bire-fringent measurements were presented.The purpose of this work is to provide a useful perspective on the characterization of birefringence for NLO materials.It is hoped that this review can give a clear description of the birefringence measurements and accelerate the discovery of new NLO crystals.展开更多
The huge discrepancies between actual devices and theoretical assumptions severely threaten the security of quantum key distribution.Recently,a general new framework called the reference technique has attracted wide a...The huge discrepancies between actual devices and theoretical assumptions severely threaten the security of quantum key distribution.Recently,a general new framework called the reference technique has attracted wide attention in defending against the imperfect sources of quantum key distribution.Here,the state preparation flaws,the side channels of mode dependencies,the Trojan horse attacks,and the pulse classical correlations are studied by using the reference technique on the phase-matching protocol.Our simulation results highlight the importance of the actual secure parameters choice for transmitters,which is necessary to achieve secure communication.Increasing the single actual secure parameter will reduce the secure key rate.However,as long as the parameters are set properly,the secure key rate is still high.Considering the influences of multiple actual secure parameters will significantly reduce the secure key rate.These actual secure parameters must be considered when scientists calibrate transmitters.This work is an important step towards the practical and secure implementation of phase-matching protocol.In the future,it is essential to study the main parameters,find out their maximum and general values,classify the multiple parameters as the same parameter,and give countermeasures.展开更多
An asymmetric quantum well （AQW） is designed to emit terahertz （THz） waves by using difference frequency generation （DFG） with the structure of GaAs/Al0.2Ga0.8As/Al0.5Ga0.sAs. The characteristics of absorption c...An asymmetric quantum well （AQW） is designed to emit terahertz （THz） waves by using difference frequency generation （DFG） with the structure of GaAs/Al0.2Ga0.8As/Al0.5Ga0.sAs. The characteristics of absorption coefficients are analysed under the parabolic and non-parabolic energy-band conditions in detail. We find that the absorption coefficients vary with the two pump optical intensities, and they reach the maxima when the pump wavelengths are given as λp1 = 9.70 μm and λp2 = 10.64 μm, respectively. Compared with non-parabolic conditions, the total absorption coefficient under parabolic conditions shows a blue shift, which is due to the increase in the energy difference between the ground and excited states. By adjusting the two pump optical intensities, the wave vector phase-matching condition inside the AQW is satisfied.展开更多
基金supported by the Office of Naval Research(ONR)MURI program under Grant No.N00014-13-1-0649the National Science Foundation(NSF,Grant No.EFMA-1542741)+2 种基金support from NSF Graduate Research Fellowship(Grant No.DGE 1106400)support from the Grants-in-Aid for Specially Promoted Research(No.25000003)by the Japan Society for the Promotion of Science(JSPS)supported by JSPS through a research fellowship for young scientists and through the Materials Education Program for the Future Leaders in Research,Industry and Technology(MERIT).
文摘Second-harmonic generation(SHG)has found extensive applications from hand-held laser pointers to spectroscopic and microscopic techniques.Recently,some cleavable van der Waals(vdW)crystals have shown SHG arising from a single atomic layer,where the SH light elucidated important information such as the grain boundaries and electronic structure in these ultra-thin materials.However,despite the inversion asymmetry of the single layer,the typical crystal stacking restores inversion symmetry for even numbers of layers leading to an oscillatory SH response,drastically reducing the applicability of vdW crystals such as molybdenum disulfide(MoS_(2)).Here,we probe the SHG generated from the noncentrosymmetric 3R crystal phase of MoS_(2).We experimentally observed quadratic dependence of second-harmonic intensity on layer number as a result of atomically phase-matched nonlinear dipoles in layers of the 3R crystal that constructively interfere.By studying the layer evolution of the A and B excitonic transitions in 3R-MoS_(2) using SHG spectroscopy,we also found distinct electronic structure differences arising from the crystal structure and the dramatic effect of symmetry and layer stacking on the nonlinear properties of these atomic crystals.The constructive nature of the SHG in this 2D crystal provides a platform to reliably develop atomically flat and controllably thin nonlinear media.
基金supported by the National Natural Science Foundation of China(Nos.12074299,11704290,and 92365106)the Guangdong Provincial Key Laboratory(No.GKLQSE202102)the Natural Science Foundation of Hubei Province(2022CFA039)。
文摘Entangled photon pairs are crucial resources for quantum information processing protocols.Via the process of spontaneous parametric downconversion(SPDC),we can generate these photon pairs using bulk nonlinear crystals.Traditionally,the crystal is designed to satisfy a specific type of phase-matching condition.Here,we report controllable transitions among different types of phase matching in a single periodically poled potassium titanyl phosphate crystal.By carefully selecting pump conditions,we can satisfy different phase-matching conditions.This allows us to observe first-order Type-II,fifth-order Type-I,third-order Type-0,and fifth-order Type-II SPDCs.The temperature-dependent spectra of our source were also analyzed in detail.Finally,we discussed the possibility of observing more than nine SPDCs in this crystal.Our work not only deepens the understanding of the physics behind phase-matching conditions,but also offers the potential for a highly versatile entangled biphoton source for quantum information research.
基金supported by the National Natural Science Foundation of China(51922014,11774414,51972336 and 61835014)the Key Research Program of Frontier Sciences,CAS(ZDBSLY-SLH035)+2 种基金Tianshan Innovation Team Program(2018D14001)the Western Light Foundation of CAS(Y92S191301)Fujian Institute of Innovation,CAS。
文摘As a promising candidate,the fluorooxoborate has enkindled new explorations of nonlinear optical materials to meet the deep-ultraviolet criteria.However,big challenges and open questions still remain facing this exciting new field,especially the birefringence and dispersion of refractive index which are fundamental parameters for determining the phasematching second harmonic generation wavelength.Here we designed possible anionic groups in fluorooxoborates,and analyzed the optical anisotropy to check its influence on birefringence,which was proved further by the response electronic distribution anisotropy approximation.The functional modules modulating birefringence in fluorooxoborates were explored systematically.We developed an approach for evaluating the behavior of the refractive index dispersions and found that the fluorooxoborates had small refractive index dispersions owing to the introduction of fluorooxoborate modules.Our results demonstrate that fluorooxoborates can be utilized to realize short phase-matching wavelength markedly and offer a path toward novel performance-driven materials design.
文摘We investigate off-axis phase-matched terahertz(THz)radiation in laser plasma pumped by few-cycle laser pulses.We find that the THz amplitude and angular distributions in the far field are sensitively dependent on the pump pulse’s focal carrier-envelope phase(CEP).Ring-like profiles of THz radiation are obtained at CEP values of 0.5πand 1.5π,due to the inversely symmetric local THz waveforms emitted before and after laser focus.Off-axis phase-matched THz radiation offers a tool to accurately measure the CEP of few-cycle pulses at the center of a medium.
基金Project supported by the National Natural Science Foundation of China (Grant Nos.12274230,91950102,and 11834004)the Funding of Nanjing University of Science and Technology (Grant No.TSXK2022D005)。
文摘The extreme ultraviolet(XUV)light beam carrying orbital angular momentum(OAM)can be produced via high-order harmonic generation(HHG)due to the interaction of an intense vortex infrared laser and a gas medium.Here we show that the OAM spectrum of vortex HHG can be readily tailored by varying the radial node(from 0 to 2)in the driving laser consisting of two mixed Laguerre-Gaussian(LG)beams.We find that due to the change in spatial profile of HHG,the distribution range of the OAM spectrum can be broadened and its shape can be modified by increasing the radial node.We also show that the OAM mode range becomes much wider and its distribution shape becomes more symmetric when the harmonic order is increased from the plateau to the cutoff when the driving laser has the nonzero radial nodes.Through the map of coherence length and the evolution of harmonic field in the medium,we reveal that the favorable off-axis phase-matching conditions are greatly modified due to the change of intensity and phase distributions of driving laser with the radial node.We anticipate this work to stimulate some interests in generating the XUV vortex beam with tunable OAM spectrum through the gaseous HHG process achieved by manipulating the mode properties of the driving laser beam.
基金supported by the National Natural Science Foundation of China(Grant No.21975062)Hebei Province Outstanding Youth Fund(Grant No.E2020201003)+1 种基金Science and Technology Project of Hebei Education Department(Grant Nos.ZD2022156,BJ2020020)Key Projects of Scientific Research and Cultivation Fund of Baoding University(Grant No.2022Z01).
文摘Nonlinear optical(NLO)materials play an increasingly important role in laser technology.Birefringence is one of the most important parameters for NLO materials to realize angle phase-matching conditions.In comparison with other desirable optical properties,the availability of birefringence and refractive index dispersion is especially problematic owing to the strict requirements for single crystals.In this review,we described how to obtain the refractive index and birefringence of NLO materials from crystals sub-millimeters to centimeters in size.Espe-cially,recently developed methods including the minimum deflection angle method,auto-collimation method,prism coupling method,oil immersion technique,interference color method,and theoretical calculation(DFT)for rapid assessment of birefringence are summarized,the contents of which are mainly focused on the principles and typical applications,together with the advantages and drawbacks.In addition,representative examples of bire-fringent measurements were presented.The purpose of this work is to provide a useful perspective on the characterization of birefringence for NLO materials.It is hoped that this review can give a clear description of the birefringence measurements and accelerate the discovery of new NLO crystals.
基金the National Key Research and Development Program of China(Grant Nos.2020YFA0309702 and 2020YFA0309701)the National Natural Science Foundation of China(Grant No.62101597)+2 种基金the China Postdoctoral Science Foundation(Grant No.2021M691536)the Natural Science Foundation of Henan(Grant Nos.202300410534 and 202300410532)the Anhui Initiative in Quantum Information Technologies。
文摘The huge discrepancies between actual devices and theoretical assumptions severely threaten the security of quantum key distribution.Recently,a general new framework called the reference technique has attracted wide attention in defending against the imperfect sources of quantum key distribution.Here,the state preparation flaws,the side channels of mode dependencies,the Trojan horse attacks,and the pulse classical correlations are studied by using the reference technique on the phase-matching protocol.Our simulation results highlight the importance of the actual secure parameters choice for transmitters,which is necessary to achieve secure communication.Increasing the single actual secure parameter will reduce the secure key rate.However,as long as the parameters are set properly,the secure key rate is still high.Considering the influences of multiple actual secure parameters will significantly reduce the secure key rate.These actual secure parameters must be considered when scientists calibrate transmitters.This work is an important step towards the practical and secure implementation of phase-matching protocol.In the future,it is essential to study the main parameters,find out their maximum and general values,classify the multiple parameters as the same parameter,and give countermeasures.
基金Project supported by the National Natural Science Foundation of China (Grant Nos. 60801017,61172010,61101058,and 61107086)the Fund from the Science and Technology Committee of Tianjin,China (Grant No. 11JCYBJC01100)
文摘An asymmetric quantum well （AQW） is designed to emit terahertz （THz） waves by using difference frequency generation （DFG） with the structure of GaAs/Al0.2Ga0.8As/Al0.5Ga0.sAs. The characteristics of absorption coefficients are analysed under the parabolic and non-parabolic energy-band conditions in detail. We find that the absorption coefficients vary with the two pump optical intensities, and they reach the maxima when the pump wavelengths are given as λp1 = 9.70 μm and λp2 = 10.64 μm, respectively. Compared with non-parabolic conditions, the total absorption coefficient under parabolic conditions shows a blue shift, which is due to the increase in the energy difference between the ground and excited states. By adjusting the two pump optical intensities, the wave vector phase-matching condition inside the AQW is satisfied.
