Observation and characterization are reported on a neutral-ionic (NI) phase
transition under pressure in (BEDT-TTF)(ClMeTCNQ), which is a mixed-stack
charge-transfer compound with BEDT-TTF-based intercolumnar networks. Optica
l and electrical experiments revealed that the compound undergoes a pressur
e-induced NI transition at 1 GPa at room temperature. The temperature-press
ure phase diagram of this phase transition was established by the electrica
l resistivity measurements at low temperature under pressure. The observed
symmetry breaking in the infrared spectra and dramatic decrease of resistiv
ity indicate that the NI transition in (BEDT-TTF)(ClMeTCNQ) at 1 GPa at roo
m temperature is qualitatively similar in nature to that in the standard ma
terial (TTF)(CA). In contrast, the NI transition in (BEDT-TTF)(ClMeTCNQ) at
low temperature under lower pressure considerably differs from that in (TT
F)(CA) as to the resistivity behaviors around the phase boundary: The forme
r becomes almost continuous without showing any anomaly, while the latter i
s significantly discontinuous. We discuss the origin of the observed electr
ical behaviors in (BEDT-TTF)(ClMeTCNQ) in terms of the effect of intercolum
nar interaction associated with BEDT-TTF moieties.