Temperature-Controlled Entangled-Photon Absorption Spectroscopy

• Published in: Physical review letters 2019-07, Vol.123 (2), p.023601-023601, Article 023601
• Main Authors: León-Montiel, Roberto de J, Svozilík, Jiří, Torres, Juan P, U'Ren, Alfred B
• Format: Article
• Language: English
• Subjects: Absorption spectroscopy; Energy levels; Enginyeria de la telecomunicació; Fotònica; Fourier transforms; Gravitational waves; Instruments; Molecular structure; Photon absorption; Photonics; Photons; Space vehicles; Spectrum analysis; Stability; Telecomunicació òptica; Àrees temàtiques de la UPC
• ISSN: 0031-9007; 1079-7114
• DOI: 10.1103/PhysRevLett.123.023601

Entangled two-photon absorption spectroscopy (TPA) has been widely recognized as a powerful tool for revealing relevant information about the structure of complex molecular systems. However, to date, the experimental implementation of this technique has remained elusive, mainly because of two major difficulties: first, the need to perform multiple experiments with two-photon states bearing different temporal correlations, which translates into the necessity to have at the experimenter's disposal tens, if not hundreds, of sources of entangled photons; second, the need to have a priori knowledge of the absorbing medium's lowest-lying intermediate energy level. In this work, we put forward a simple experimental scheme that successfully overcomes these two limitations. By making use of a temperature-controlled entangled-photon source, which allows the tuning of the central frequencies of the absorbed photons, we show that the TPA signal, measured as a function of the temperature of the nonlinear crystal that generates the paired photons, and a controllable delay between them, carries all information about the electronic level structure of the absorbing medium, which can be revealed by a simple Fourier transformation.