论文标题

在任意延迟间隔内,速扫的非线性时间分辨光谱

Rapid-scan nonlinear time-resolved spectroscopy over arbitrary delay intervals

论文作者

Flöry, Tobias, Stummer, Vinzenz, Pupeikis, Justinas, Willenberg, Benjamin, Nussbaum-Lapping, Alexander, Camargo, Franco V. A., Barkauskas, Martynas, Phillips, Christopher, Keller, Ursula, Cerullo, Giulio, Pugzlys, Audrius, Baltuska, Andrius

论文摘要

飞秒双弯曲激光器通过提供快速运动,精确和准确的测量模式,并在RF域中易于注册,彻底改变了线性傅立叶域光谱。该技术的扩展发现已经在以全振荡器重复速率运行的来源可用的能量限制内应用了非线性时间分辨光谱。在这里,我们提出了一种基于激光放大器中脉冲门控为飞秒频率梳的时间过滤的技术。这为脉搏能提供了所需的提升,并为泵探针技术的一对任意延迟的波长脉冲脉冲提供了灵活性。使用双通道Millijoule放大器,我们展示了非常短,FS和极长(> ns)插入式延迟的可编程生成。可以在每个连续的放大器拍摄中直接实现预定的任意选择的插孔延迟,从而消除了通过光学机械线或两个自由运行振荡器的异步扫描更改延迟设置所需的大量等待时间。我们通过测量CHI^(2)互相关和CHI^(3)多组分种群恢复动力学来确认这种延迟生成方法的多功能性。

Femtosecond dual-comb lasers have revolutionized linear Fourier-domain spectroscopy by offering a rapid motion-free, precise and accurate measurement mode with easy registration of the combs beat note in the RF domain. Extensions of this technique found already application for nonlinear time-resolved spectroscopy within the energy limit available from sources operating at the full oscillator repetition rate. Here, we present a technique based on time filtering of femtosecond frequency combs by pulse gating in a laser amplifier. This gives the required boost to the pulse energy and provides the flexibility to engineer pairs of arbitrarily delayed wavelength-tunable pulses for pump-probe techniques. Using a dual-channel millijoule amplifier, we demonstrate programmable generation of both extremely short, fs, and extremely long (>ns) interpulse delays. A predetermined arbitrarily chosen interpulse delay can be directly realized in each successive amplifier shot, eliminating the massive waiting time required to alter the delay setting by means of an optomechanical line or an asynchronous scan of two free-running oscillators. We confirm the versatility of this delay generation method by measuring chi^(2) cross-correlation and chi^(3) multicomponent population recovery kinetics.

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