论文标题

通过振动辅助发光单分子中IR检测

Single-molecule mid-IR detection through vibrationally-assisted luminescence

论文作者

Chikkaraddy, Rohit, Arul, Rakesh, Jakob, Lukas A., Baumberg, Jeremy J.

论文摘要

中红外分子振动的室温检测(mir,$λ$ = 3-30 $μ$ m)具有许多应用,包括实时气体感应,化学反应性,医学成像,天文学调查和量子通信[1,2]。然而,热噪声严重阻碍了miR检测,因此当前技术依赖于能量密集的冷却半导体探测器(Mercury cadmium telluride,MCT)[3,4,5]。克服这一挑战的一种方法是将低能量的mir光升至高能可见波长($λ$ = 500-800nm),其中使用硅技术很容易实现单个光子的检测[6,7]。这个过程遭受了较弱的横截面以及MIR和可见波长之间的不匹配,从而限制了其效率。在这里,我们利用具有MiR和可见过渡的分子发射器,从分子振动和电子状态下,并通过Frank-Condon因子耦合。通过将分子组装到纳米级腔中,并连续将它们泵入电子吸收带的下方,我们显示了通过分子振动吸收的miR光的转导。向上转化的信号被观察到增强的高能发光。将purcell增强的可见发光与增强的振动泵送速率相结合的转导效率超过10%。通过将腔体积低于$ 1NM^3 $,我们显示了对任何先前检测器无法接近的单分子债券的miR检测。

Room temperature detection of molecular vibrations in the mid-infrared (MIR, $λ$ =3-30$μ$m) has numerous applications including real-time gas sensing, chemical reactivity, medical imaging, astronomical surveys, and quantum communication [1,2]. However, MIR detection is severely hindered by thermal noise, hence current technologies rely on energy-intensive cooled semiconductor detectors (mercury cadmium telluride, MCT) [3,4,5]. One way to overcome this challenge is to upconvert the low-energy MIR light into high-energy visible wavelengths ($λ$ =500-800nm) where detection of single photons is easily achieved using silicon technologies [6,7]. This process suffers from weak cross sections and the mismatch between MIR and visible wavelengths, limiting its efficiency. Here, we exploit molecular emitters possessing both MIR and visible transitions from molecular vibrations and electronic states, coupled through Frank-Condon factors. By assembling molecules into a nanoscale cavity and continuously optically pumping them below the electronic absorption band, we show the transduction of MIR light absorbed by the molecular vibrations. The upconverted signal is observed as enhanced high-energy luminescence. Combining Purcell-enhanced visible luminescence with enhanced rates of vibrational pumping gives transduction efficiencies exceeding 10%. By down-scaling the cavity volume below $1nm^3$, we show MIR detection of single-molecular bonds, inaccessible to any previous detector.

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