碳化铁θ-Fe_(3)C作为费托反应活性相之一,其氧化造成了催化剂的严重失活。探究氧原子在碳化铁晶面的吸附及移除机理有助于理解氧化过程,为提高催化剂的稳定性提供参考。本工作通过理论计算研究了低覆盖度下氧原子在θ-Fe_(3)C不同晶面...碳化铁θ-Fe_(3)C作为费托反应活性相之一,其氧化造成了催化剂的严重失活。探究氧原子在碳化铁晶面的吸附及移除机理有助于理解氧化过程,为提高催化剂的稳定性提供参考。本工作通过理论计算研究了低覆盖度下氧原子在θ-Fe_(3)C不同晶面的吸附,其在(110)晶面吸附最强,(001)晶面次之,(011)晶面吸附最弱,即(110)容易氧化。原子热力学研究表明,增大H_(2)O分压或降低温度有利于氧原子吸附,容易造成表面氧化。此外,在典型费托反应条件下(110)晶面氧原子的覆盖度最高,进一步证明该晶面易氧化,与低覆盖度吸附结果一致。对移除路径进行计算得出,(011)晶面吸附氧原子直接与CO反应以CO_(2)方式移除能垒较低(0.84 eV);(001)与(110)晶面吸附氧原子主要通过OH歧化以H_(2)O方式移除,但后者形成O−H键需要克服的能垒更高(1.72 vs 1.47 eV)。展开更多
We study the energy scaling of terahertz (THz) emission through difference frequency generation of near-infrared pulses, and demonstrate that Gigawatt few-cycle THz transients at the central frequency of 30 THz are pr...We study the energy scaling of terahertz (THz) emission through difference frequency generation of near-infrared pulses, and demonstrate that Gigawatt few-cycle THz transients at the central frequency of 30 THz are produced from GaSe crystal pumped by two pulses at 1.65 and 1.95 micrometers, with the high quantum yield of 28%. Our analysis indicates that the high yield of DFG originates from the largely reduced group velocity mismatch as the long-wavelength pumping pulses are employed.展开更多
We experimentally investigate the evolution of the terahertz（THz） waveform and polarization state inside the plasma filament produced by orthogonally polarized two-color pulses. We find that the variation of the THz...We experimentally investigate the evolution of the terahertz（THz） waveform and polarization state inside the plasma filament produced by orthogonally polarized two-color pulses. We find that the variation of the THz polarization state along the plasma column is dominantly caused by the relative phase difference and spectra blue shift of the two-color field. Elliptically polarized THz radiation is generated by controlling the initial relative phase and the filament length. The result indicates the coherent control of the polarization state of the THz emission.展开更多
We present a velocity-gauge model for the generation of even-order high harmonics, and reveal that the even-order harmonics originate from the multiple-step transitions among the energy bands in momentum space, while ...We present a velocity-gauge model for the generation of even-order high harmonics, and reveal that the even-order harmonics originate from the multiple-step transitions among the energy bands in momentum space, while the odd-order harmonics are mainly from direct transitions. The lower valence band is found vital for the generation of even harmonics. Relative intensity of even-order harmonics versus the odd orders is calculated and shows a growing trend as the laser field amplitude increases.展开更多
基金National Natural Science Foundation of China (Nos.11874373,12174412,12174413)Youth Innovation Promotion Association of the Chinese Academy of Sciences (No.2021241)+1 种基金Scientific Instrument Developing Project of the Chinese Academy of Sciences (No.YJKYYQ20180023)the CAS Project for Young Scientists in Basic Research (No.YSBR-091)。
文摘碳化铁θ-Fe_(3)C作为费托反应活性相之一,其氧化造成了催化剂的严重失活。探究氧原子在碳化铁晶面的吸附及移除机理有助于理解氧化过程,为提高催化剂的稳定性提供参考。本工作通过理论计算研究了低覆盖度下氧原子在θ-Fe_(3)C不同晶面的吸附,其在(110)晶面吸附最强,(001)晶面次之,(011)晶面吸附最弱,即(110)容易氧化。原子热力学研究表明,增大H_(2)O分压或降低温度有利于氧原子吸附,容易造成表面氧化。此外,在典型费托反应条件下(110)晶面氧原子的覆盖度最高,进一步证明该晶面易氧化,与低覆盖度吸附结果一致。对移除路径进行计算得出,(011)晶面吸附氧原子直接与CO反应以CO_(2)方式移除能垒较低(0.84 eV);(001)与(110)晶面吸附氧原子主要通过OH歧化以H_(2)O方式移除,但后者形成O−H键需要克服的能垒更高(1.72 vs 1.47 eV)。
基金Supported by the National Natural Science Foundation of China under Grant Nos 11274326,61221064,61405222,11134010 and 11127901the Shanghai Sailing Program under Grant No 14YF1406200
文摘We study the energy scaling of terahertz (THz) emission through difference frequency generation of near-infrared pulses, and demonstrate that Gigawatt few-cycle THz transients at the central frequency of 30 THz are produced from GaSe crystal pumped by two pulses at 1.65 and 1.95 micrometers, with the high quantum yield of 28%. Our analysis indicates that the high yield of DFG originates from the largely reduced group velocity mismatch as the long-wavelength pumping pulses are employed.
基金supported by the National Science Foundation of China(Nos.11274326,61221064,61405222,61505234,11134010,and 11127901)the Shanghai Sailing Program(No.14YF1406200)the National 973 Program of China(No.2011CB808103)
文摘We experimentally investigate the evolution of the terahertz（THz） waveform and polarization state inside the plasma filament produced by orthogonally polarized two-color pulses. We find that the variation of the THz polarization state along the plasma column is dominantly caused by the relative phase difference and spectra blue shift of the two-color field. Elliptically polarized THz radiation is generated by controlling the initial relative phase and the filament length. The result indicates the coherent control of the polarization state of the THz emission.
基金supported by the National Natural Science Foundation of China (NSFC) (Nos. 11127901, 11134010, 61221064, and 61405222)the Strategic Priority Research Program of Chinese Academy of Sciences (CAS) (No. XDB16000000)。
文摘We present a velocity-gauge model for the generation of even-order high harmonics, and reveal that the even-order harmonics originate from the multiple-step transitions among the energy bands in momentum space, while the odd-order harmonics are mainly from direct transitions. The lower valence band is found vital for the generation of even harmonics. Relative intensity of even-order harmonics versus the odd orders is calculated and shows a growing trend as the laser field amplitude increases.
