Time-resolved spectroscopies using intense THz pulses appear as a promising tool to address collective electronic excitations in condensed matter. In particular, recent experiments showed the possibility to selectively excite collective modes emerging across a phase transition, as is the case for superconducting and charge-density-wave (CDW) systems. One possible signature of these excitations is the emergence of coherent oscillations of the differential probe field in pump-probe protocols. While the analogy with the case of phonon modes suggests that the basic underlying mechanism should be a sum-frequency stimulated Raman process, a general theoretical scheme able to describe the experiments and to define the relevant optical quantity is still lacking. Here we provide this scheme by showing that coherent oscillations as a function of the pump-probe time delay can be linked to the convolution in the frequency domain between the squared pump field and a Raman-like nonlinear optical kernel. This approach is applied and discussed in a few paradigmatic examples: Ordinary phonons in an insulator, and collective charge and Higgs fluctuations across a superconducting and a CDW transition. Our results not only account very well for the existing experimental data in a wide variety of systems, but they also offer a useful perspective to design future experiments in emerging materials.
Theory of coherent-oscillations generation in terahertz pump-probe spectroscopy: From phonons to electronic collective modes
Udina M.;Benfatto L.
2019
Abstract
Time-resolved spectroscopies using intense THz pulses appear as a promising tool to address collective electronic excitations in condensed matter. In particular, recent experiments showed the possibility to selectively excite collective modes emerging across a phase transition, as is the case for superconducting and charge-density-wave (CDW) systems. One possible signature of these excitations is the emergence of coherent oscillations of the differential probe field in pump-probe protocols. While the analogy with the case of phonon modes suggests that the basic underlying mechanism should be a sum-frequency stimulated Raman process, a general theoretical scheme able to describe the experiments and to define the relevant optical quantity is still lacking. Here we provide this scheme by showing that coherent oscillations as a function of the pump-probe time delay can be linked to the convolution in the frequency domain between the squared pump field and a Raman-like nonlinear optical kernel. This approach is applied and discussed in a few paradigmatic examples: Ordinary phonons in an insulator, and collective charge and Higgs fluctuations across a superconducting and a CDW transition. Our results not only account very well for the existing experimental data in a wide variety of systems, but they also offer a useful perspective to design future experiments in emerging materials.File | Dimensione | Formato | |
---|---|---|---|
prod_409389-doc_143918.pdf
solo utenti autorizzati
Descrizione: Theory of coherent-oscillations generation in terahertz pump-probe spectroscopy
Tipologia:
Versione Editoriale (PDF)
Licenza:
NON PUBBLICO - Accesso privato/ristretto
Dimensione
2.18 MB
Formato
Adobe PDF
|
2.18 MB | Adobe PDF | Visualizza/Apri Richiedi una copia |
I documenti in IRIS sono protetti da copyright e tutti i diritti sono riservati, salvo diversa indicazione.